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Sample records for minor uranium isotopes

  1. Increasing the Accuracy in the Measurement of the Minor Isotopes of Uranium: Care in Selection of Reference Materials, Baselines and Detector Calibration

    NASA Astrophysics Data System (ADS)

    Poths, J.; Koepf, A.; Boulyga, S. F.

    2008-12-01

    The minor isotopes of uranium (U-233, U-234, U-236) are increasingly useful for tracing a variety of processes: movement of anthropogenic nuclides in the environment (ref 1), sources of uranium ores (ref 2), and nuclear material attribution (ref 3). We report on improved accuracy for U-234/238 and U-236/238 by supplementing total evaporation protocol TIMS measurement on Faraday detectors (ref 4)with multiplier measurement for the minor isotopes. Measurement of small signals on Faraday detectors alone is limited by noise floors of the amplifiers and accurate measurement of the baseline offsets. The combined detector approach improves the reproducibility to better than ±1% (relative) for the U-234/238 at natural abundance, and yields a detection limit for U-236/U-238 of <0.2 ppm. We have quantified contribution of different factors to the uncertainties associated with these peak jumping measurement on a single detector, with an aim of further improvement. The uncertainties in the certified values for U-234 and U-236 in the uranium standard NBS U005, if used for mass bias correction, dominates the uncertainty in their isotopic ratio measurements. Software limitations in baseline measurement drives the detection limit for the U-236/U-238 ratio. This is a topic for discussion with the instrument manufacturers. Finally, deviation from linearity of the response of the electron multiplier with count rate limits the accuracy and reproducibility of these minor isotope measurements. References: (1) P. Steier et al(2008) Nuc Inst Meth(B), 266, 2246-2250. (2) E. Keegan et al (2008) Appl Geochem 23, 765-777. (3) K. Mayer et al (1998) IAEA-CN-98/11, in Advances in Destructive and Non-destructive Analysis for Environmental Monitoring and Nuclear Forensics. (4) S. Richter and S. Goldberg(2003) Int J Mass Spectrom, 229, 181-197.

  2. The terrestrial uranium isotope cycle

    NASA Astrophysics Data System (ADS)

    Andersen, Morten B.; Elliott, Tim; Freymuth, Heye; Sims, Kenneth W. W.; Niu, Yaoling; Kelley, Katherine A.

    2015-01-01

    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 238U/235U ratios, as a result of alteration processes at the bottom of an oxic ocean. We also find that mid-ocean-ridge basalts (MORBs) have 238U/235U 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.

  3. The terrestrial uranium isotope cycle.

    PubMed

    Andersen, Morten B; Elliott, Tim; Freymuth, Heye; Sims, Kenneth W W; Niu, Yaoling; Kelley, Katherine A

    2015-01-15

    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. PMID:25592542

  4. Ultratrace Uranium Fingerprinting with Isotope Selective Laser Ionization Spectrometry

    SciTech Connect

    Ziegler, Summer L.; Bushaw, Bruce A.

    2008-08-01

    Uranium isotope ratios can provide source information for tracking uranium contamination in a variety of fields, ranging from occupational bioassay to monitoring aftereffects of nuclear accidents. We describe the development of Isotope Selective Laser Ionization Spectrometry (ISLIS) for ultratrace measurement of the minor isotopes 234U, 235U, and 236U with respect to 238U. Optical isotopic selectivity in three-step excitation with single-mode continuous wave lasers is capable of measuring the minor isotopes at relative abundances below 1 ppm, and is not limited by isobaric interferences such as 235UH+ during measurement of 236U. This relative abundance limit approaches the threshold for measurement of uranium minor isotopes with conventional mass spectrometry, typically 10-7, but without mass spectrometric analysis of the laser-created ions. Uranyl nitrate standards from an international blind comparison were used to test analytical performance for different isotopic compositions and with quantities ranging from 11 ng to 10 µg total uranium. Isotopic ratio determination was demonstrated over a linear dynamic range of 7 orders of magnitude with a few percent relative precision and detection limits below 500 fg for the minor isotopes.

  5. NUSIMEP-7: uranium isotope amount ratios in uranium particles.

    PubMed

    Truyens, J; Stefaniak, E A; Aregbe, Y

    2013-11-01

    The Institute for Reference Materials and Measurements (IRMM) has extensive experience in the development of isotopic reference materials and the organization of interlaboratory comparisons (ILC) for nuclear measurements in compliance with the respective international guidelines (ISO Guide 34:2009 and ISO/IEC 17043:2010). The IRMM Nuclear Signatures Interlaboratory Measurement Evaluation Program (NUSIMEP) is an external quality control program with the objective of providing materials for measurements of trace amounts of nuclear materials in environmental matrices. Measurements of the isotopic ratios of the elements uranium and plutonium in small amounts, typical of those found in environmental samples, are required for nuclear safeguards and security, for the control of environmental contamination and for the detection of nuclear proliferation. The measurement results of participants in NUSIMEP are evaluated according to international guidelines in comparison to independent external certified reference values with demonstrated metrological traceability and uncertainty. NUSIMEP-7 focused on measurements of uranium isotope amount ratios in uranium particles aiming to support European Safeguards Directorate General for Energy (DG ENER), the International Atomic Energy Agency's (IAEA) network of analytical laboratories for environmental sampling (NWAL) and laboratories in the field of particle analysis. Each participant was provided two certified test samples: one with single and one with double isotopic enrichment. These NUSIMEP test samples were prepared by controlled hydrolysis of certified uranium hexafluoride in a specially designed aerosol deposition chamber at IRMM. Laboratories participating in NUSIMEP-7 received the test samples of uranium particles on two graphite disks with undisclosed isotopic ratio values n((234)U)/n((238)U), n((235)U)/n((238)U) and n((236)U)/n((238)U). The uranium isotope ratios had to be measured using their routine analytical

  6. Ultratrace uranium fingerprinting with isotope selective laser ionization spectrometry.

    PubMed

    Ziegler, Summer L; Bushaw, Bruce A

    2008-08-01

    Uranium isotope ratios can provide source information for tracking uranium contamination in a variety of fields, ranging from occupational bioassay to monitoring aftereffects of nuclear accidents. We describe the development of isotope selective laser ionization spectrometry for ultratrace measurement of the minor isotopes (234)U, (235)U, and (236)U with respect to (238)U. The inherent isotopic selectivity of three-step excitation with single-mode continuous wave lasers results in measurement of the minor isotopes at relative abundances below 1 ppm and is not limited by isobaric interferences such as (235)UH(+) during measurement of (236)U. This relative abundance limit is attained without mass spectrometric analysis of the laser-created ions. Uranyl nitrate standards from an international blind comparison were used to test analytical performance for different isotopic compositions and with quantities ranging from 11 ng to 10 microg total uranium. Isotopic ratio determination was demonstrated over a linear dynamic range of 7 orders of magnitude with a few percent relative precision and detection limits below 500 fg for the minor isotopes. PMID:18613650

  7. Uranium isotopes fingerprint biotic reduction

    SciTech Connect

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

    2015-04-20

    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. In addition, 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.

  8. Uranium isotopes fingerprint biotic reduction

    DOE PAGESBeta

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

    2015-04-20

    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),more » 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. In addition, 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.« less

  9. Uranium isotopes fingerprint biotic reduction.

    PubMed

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

    2015-05-01

    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

  10. Uranium isotopes fingerprint biotic reduction

    PubMed Central

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

    2015-01-01

    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

  11. Isotopic Compositions of Uranium Reference Materials

    NASA Astrophysics Data System (ADS)

    Jacobsen, B.; Borg, L. E.; Williams, R. W.; Brennecka, G.; Hutcheon, I. D.

    2009-12-01

    Uranium isotopic compositions of a variety of U standard materials were measured at Lawrence Livermore National Laboratory and are reported here. Both thermal ionization mass spectrometry (TIMS) and multi-collector inductively couple plasma mass spectrometry (MC-ICPMS) were used to determine ratios of the naturally occurring isotopes of U. Establishing an internally coherent set of isotopic values for a range of U standards is essential for inter-laboratory comparison of small differences in 238U/235U, as well as the minor isotopes of U. Differences of ~1.3‰ are now being observed in 238U/235U in natural samples, and may play an important role in understanding U geochemistry where tracing the origin of U is aided by U isotopic compositions. The 238U/235U ratios were measured with a TRITON TIMS using a mixed 233U-236U isotopic tracer to correct for instrument fractionation. This tracer was extremely pure and resulted in only very minor corrections on the measured 238U/235U ratios of ~0.03. The values obtained for 238U/235U are: IRMM184 = 137.698 ± 0.020 (n=15), SRM950a = 137.870 ± 0.018 (n=8), and CRM112a = 137.866 ± 0.030 (n=16). Uncertainties represent 2 s.d. of the population. Our measured value for IRMM184 is in near-perfect agreement with the certified value of 137.697 ± 0.042. However, the U isotopic compositions of SRM950a and CRM112a are not certified. Minor isotopes of U were determined with a Nu Plasma HR MC-ICPMS and mass bias was corrected by sample/standard bracketing to IRMM184, using its certified 238U/235U ratio. Thus, the isotopic compositions determined using both instruments are compatible. The values obtained for 234U/235U are: SRM950a = (7.437 ± 0.043)x10-3 (n=18), and CRM112a = (7.281 ± 0.050)x10-3 (n=16), both of which are in good agreement with published values. The value for 236U/235U in SRM950a was determined to be (8.48 ± 2.63)x10-6, whereas 236U was not detected in CRM112a. We are currently obtaining the U isotopic composition of

  12. ISOTOPIC COMPOSITIONS OF URANIUM REFERENCE MATERIALS

    SciTech Connect

    Jacobsen, B; Borg, L; Williams, R; Brennecka, G; Hutcheon, I

    2009-09-03

    Uranium isotopic compositions of a variety of U standard materials were measured at Lawrence Livermore National Laboratory and are reported here. Both thermal ionization mass spectrometry (TIMS) and multi-collector inductively couple plasma mass spectrometry (MC-ICPMS) were used to determine ratios of the naturally occurring isotopes of U. Establishing an internally coherent set of isotopic values for a range of U standards is essential for inter-laboratory comparison of small differences in {sup 238}U/{sup 235}U, as well as the minor isotopes of U. Differences of {approx} 1.3{per_thousand} are now being observed in {sup 238}U/{sup 235}U in natural samples, and may play an important role in understanding U geochemistry where tracing the origin of U is aided by U isotopic compositions. The {sup 238}U/{sup 235}U ratios were measured with a TRITON TIMS using a mixed {sup 233}U-{sup 236}U isotopic tracer to correct for instrument fractionation. this tracer was extremely pure and resulted in only very minor corrections on the measured {sup 238}U/{sup 235}U ratios of {approx} 0.03. The values obtained for {sup 238}U/{sup 235}U are: IRMM184 = 137.698 {+-} 0.020 (n = 15), SRM950a = 137.870 {+-} 0.018 (n = 8), and CRM112a = 137.866 {+-} 0.030 (n = 16). Uncertainties represent 2 s.d. of the population. The measured value for IRMM184 is in near-perfect agreement with the certified value of 137.697 {+-} 0.042. However, the U isotopic compositions of SRM950a and CRM112a are not certified. Minor isotopes of U were determined with a Nu Plasma HR MC-ICPMS and mass bias was corrected by sample/standard bracketing to IRMM184, using its certified {sup 238}U/{sup 235}U ratio. Thus, the isotopic compositions determined using both instruments are compatible. The values obtained for {sup 234}U/{sup 235}U are: SRM950a = (7.437 {+-} 0.043) x 10{sup -3} (n = 18), and CRM112a = (7.281 {+-} 0.050) x 10{sup -3} (n = 16), both of which are in good agreement with published values. The value for

  13. Uranium Isotopic Analysis with the FRAM Isotopic Analysis Code

    SciTech Connect

    Duc T. Vo; Thomas E. Sampson

    1999-05-01

    FRAM is the acronym for Fixed-energy Response-function Analysis with Multiple efficiency. This software was developed at Los Alamos National Laboratory originally for plutonium isotopic analysis. Later, it was adapted for uranium isotopic analysis in addition to plutonium. It is a code based on a self-calibration using several gamma-ray peaks for determining the isotopic ratios. The versatile-parameter database structure governs all facets of the data analysis. User editing of the parameter sets allows great flexibility in handling data with different isotopic distributions, interfering isotopes, and different acquisition parameters such as energy calibration and detector type.

  14. Uranium and plutonium isotopes in the atmosphere

    SciTech Connect

    Sakuragi, Y.; Meason, J.L.; Kuroda, P.K.

    1983-04-20

    Uranium 234 and 235 were found to be highly enriched relative to uranium 238 in several rain samples collected at Fayetteville, Arkansas, during the months of April and May 1980. The anomalous uranium appears to have originated from the Soviet satellite Cosmos-954, which fell over Canada on January 24, 1978. The uranium fallout occurred just about the time Mount St. Helens erupted on May 18, 1980. The concentration of /sup 238/U in rain increased markedly after the eruption of Mount St. Helens, and it appeared as if a large quantity of natural uranium was injected into the atmosphere by the volcanic eruption. The pattern of variation of the concentrations of uranium in rain after the eruption of Mount St. Helens was found to be similar to that of plutonium isotopes.

  15. AMS of the Minor Plutonium Isotopes.

    PubMed

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

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure (239)Pu, (240)Pu, (241)Pu, (242)Pu and (244)Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of (244)Pu/(239)Pu = (5.7 ± 1.0) × 10(-5) based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the (242)Pu/(240)Pu ratio as an estimate of the initial (241)Pu/(239)Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method. PMID:23565016

  16. AMS of the Minor Plutonium Isotopes

    PubMed Central

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

    2013-01-01

    VERA, the Vienna Environmental Research Accelerator, is especially equipped for the measurement of actinides, and performs a growing number of measurements on environmental samples. While AMS is not the optimum method for each particular plutonium isotope, the possibility to measure 239Pu, 240Pu, 241Pu, 242Pu and 244Pu on the same AMS sputter target is a great simplification. We have obtained a first result on the global fallout value of 244Pu/239Pu = (5.7 ± 1.0) × 10−5 based on soil samples from Salzburg prefecture, Austria. Furthermore, we suggest using the 242Pu/240Pu ratio as an estimate of the initial 241Pu/239Pu ratio, which allows dating of the time of irradiation based solely on Pu isotopes. We have checked the validity of this estimate using literature data, simulations, and environmental samples from soil from the Salzburg prefecture (Austria), from the shut down Garigliano Nuclear Power Plant (Sessa Aurunca, Italy) and from the Irish Sea near the Sellafield nuclear facility. The maximum deviation of the estimated dates from the expected ages is 6 years, while relative dating of material from the same source seems to be possible with a precision of less than 2 years. Additional information carried by the minor plutonium isotopes may allow further improvements of the precision of the method. PMID:23565016

  17. Investigating Uranium Isotopic Distributions in Environmental Samples Using AMS and MC-ICPMS

    SciTech Connect

    Buchholz, B A; Brown, T A; Hamilton, T F; Hutcheon, I D; Marchetti, A A; Martinelli, R E; Ramon, E C; Tumey, S J; Williams, R W

    2005-12-09

    Major, minor, and trace uranium isotopes were measured at Lawrence Livermore National Laboratory in environmentally acquired samples using different instruments to span large variations in concentrations. Multi-collector inductively-coupled plasma mass spectrometry (MC-ICPMS) can be used to measure major and minor isotopes: {sup 238}U, {sup 235}U, {sup 234}U and {sup 236}U. Accelerator mass spectrometry (AMS) can be used to measure minor and trace isotopes: {sup 234}U, {sup 236}U, and {sup 233}U. The main limit of quantification for minor or trace uranium isotopes is the abundance sensitivity of the measurement technique; i.e., the ability to measure a minor or trace isotope of mass M in the presence of a major isotope at M{+-}1 mass units. The abundance sensitivity for {sup 236}U/{sup 235}U isotope ratio measurements using MC-ICPMS is around {approx}2x10{sup -6}. This compares with a {sup 236}U/{sup 235}U abundance sensitivity of {approx}1x10{sup -7} for the current AMS system, with the expectation of 2-3 orders of magnitude improvement in sensitivity with the addition of another high energy filter. Comparing {sup 236}U/{sup 234}U from MC-ICPMS and AMS produced agreement within {approx}10% for samples at {sup 236}U levels high enough to be measurable by both techniques.

  18. Investigating uranium isotopic distributions in environmental samples using AMS and MC-ICPMS

    NASA Astrophysics Data System (ADS)

    Buchholz, B. A.; Brown, T. A.; Hamilton, T. F.; Hutcheon, I. D.; Marchetti, A. A.; Martinelli, R. E.; Ramon, E. C.; Tumey, S. J.; Williams, R. W.

    2007-06-01

    Major, minor and trace uranium isotopes were measured at Lawrence Livermore National Laboratory in environmentally acquired samples using different instruments to span large variations in concentrations. Multi-collector inductively-coupled plasma mass spectrometry (MC-ICPMS) can be used to measure major and minor isotopes: 238U, 235U, 234U and 236U. Accelerator mass spectrometry (AMS) can be used to measure minor and trace isotopes: 234U, 236U and 233U. The main limit of quantification for minor or trace uranium isotopes is the abundance sensitivity of the measurement technique; i.e. the ability to measure a minor or trace isotope of mass M in the presence of a major isotope at M ± 1 mass units. The abundance sensitivity for 236U/235U isotope ratio measurements using MC-ICPMS is around ∼2 × 10-6. This compares with a 236U/235U abundance sensitivity of ∼1 × 10-7 for the current AMS system, with the expectation of 2-3 orders of magnitude improvement in sensitivity with the addition of another high energy filter. Comparing 236U/234U from MC-ICPMS and AMS produced agreement within ∼10% for samples at 236U levels high enough to be measurable by both techniques.

  19. Isotopic fractionation of uranium in sandstone

    USGS Publications Warehouse

    Rosholt, J.N.; Shields, W.R.; Garner, E.L.

    1963-01-01

    Relatively unoxidized black uranium ores from sandstone deposits in the western United States show deviations in the uranium-235 to uranium-234 ratio throughout a range from 40 percent excess uranium-234 to 40 percent deficient uranium-234 with respect to a reference uranium-235 to uranium-234 ratio. The deficient uranium-234 is leached preferentially to uranium-238 and the excess uranium-234 is believed to result from deposition of uranium-234 enriched in solutions from leached deposits.

  20. Advances in Multicollector ICPMS for precise and accurate isotope ratio measurements of Uranium isotopes

    NASA Astrophysics Data System (ADS)

    Bouman, C.; Lloyd, N. S.; Schwieters, J.

    2011-12-01

    The accurate and precise determination of uranium isotopes is challenging, because of the large dynamic range posed by the U isotope abundances and the limited available sample material. Various mass spectrometric techniques are used for the measurement of U isotopes, where TIMS is the most accepted and accurate one. Multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) can offer higher productivity compared to TIMS, but is traditionally limited by low efficiency of sample utilisation. This contribution will discuss progress in MC-ICPMS for detecting 234U, 235U, 236U and 238U in various uranium reference materials from IRMM and NBL. The Thermo Scientific NEPTUNE Plus with Jet Interface offers a modified dry plasma ICP interface using a large interface pump combined with a special set of sample and skimmer cones giving ultimate sensitivity for all elements across the mass range. For uranium, an ion yield of > 3 % was reported previously [1]. The NEPTUNE Plus also offers Multi Ion Counting using discrete dynode electron multipliers as well as two high abundance-sensitivity filters to discriminate against peak tailing effects on 234U and 236U originating from the major uranium beams. These improvements in sensitivity and dynamic range allow accurate measurements of 234U, 235U and 236U abundances on very small samples and at low concentration. In our approach, minor U isotopes 234U and 236U were detected on ion counters with high abundance sensitivity filters, whereas 235U and 238U were detected on Faraday Cups using a high gain current amplifier (10e12 Ohm) for 235U. Precisions and accuracies for 234U and 236U were down to ~1%. For 235U, subpermil levels were reached.

  1. Uranium isotope ratio measurements in field settings

    SciTech Connect

    Shaw, R.W.; Barshick, C.M.; Young, J.P.; Ramsey, J.M.

    1997-06-01

    The authors have developed a technique for uranium isotope ratio measurements of powder samples in field settings. Such a method will be invaluable for environmental studies, radioactive waste operations, and decommissioning and decontamination operations. Immediate field data can help guide an ongoing sampling campaign. The measurement encompasses glow discharge sputtering from pressed sample hollow cathodes, high resolution laser spectroscopy using conveniently tunable diode lasers, and optogalvanic detection. At 10% {sup 235}U enrichment and above, the measurement precision for {sup 235}U/({sup 235}U+{sup 238}U) isotope ratios was {+-}3%; it declined to {+-}15% for 0.3% (i.e., depleted) samples. A prototype instrument was constructed and is described.

  2. Determination of the concentration and isotopic composition of uranium in environmental air filters

    SciTech Connect

    Russ, G.P. III; Bazan, J.M.

    1994-08-26

    For many years, Lawrence Livermore National Laboratory has collected monthly air-particulate filter samples from a variety of environmental monitoring stations on and off site. Historically the concentration and isotopic composition of uranium collected on these filters was determined by isotope dilution using a {sup 233}U spike and thermal ionization mass spectrometry (TIMS). For samples containing as little as 10 nanograms of uranium, ICP-MS is now used to make these measurements to the required level of precision, about 5% in the measured 235/238 and 233/238. Unless particular care is taken to control bias in the mass filter, variable mass bias limits accuracy to a few percent. Measurements of the minor isotopes 236 (if present) and 234 are also possible and provide useful information for identifying the source of the uranium. The advantage of ICP-MS is in rapid analysis, {approximately}12 minutes of instrument time per sample.

  3. Discovery of actinium, thorium, protactinium, and uranium isotopes

    NASA Astrophysics Data System (ADS)

    Fry, C.; Thoennessen, M.

    2013-05-01

    Thirty-one actinium, thirty-one thorium, twenty-eight protactinium, and twenty-three uranium isotopes have so far been observed; the discovery of these isotopes is described. For each isotope a brief summary of the first refereed publication, including the production and identification method, is presented.

  4. Evaluating the status of uranium isotope ratio measurements using an inter-laboratory comparison campaign

    NASA Astrophysics Data System (ADS)

    Richter, S.; Alonso, A.; Truyens, J.; Kühn, H.; Verbruggen, A.; Wellum, R.

    2007-07-01

    The REIMEP 18 (Regular European Inter-laboratory Measurement Evaluation Programme) campaign for the measurement isotopic ratios of uranium in nitric acid solution was completed in December 2006. The task for all participating laboratories was to measure the uranium isotopic composition of four uranium samples ranging from depleted to slightly enriched uranium. With 71 participating laboratories REIMEP 18 has become the largest nuclear isotopic measurement campaign organized by IRMM so far. Participation in this kind of measurement campaign is an integral part of the external quality control required for nuclear safeguards laboratories worldwide. For the first time also a significant number of academic laboratories, mainly from the geochemistry area was included. Certification measurements were carried out at IRMM using state-of-the-art mass spectrometric methodology. A MAT511 UF6-gas source mass spectrometer (GSMS) was used to determine the n(235U)/n(238U) ratios and a TRITON thermal-ionization mass-spectrometer (TIMS) for the minor isotope ratios n(234U)/n(238U) and n(236U)/n(238U). Verification measurements on ampouled samples were performed successfully prior to sample shipping and showed good agreement with the certified ratios. The results of the REIMEP 18 campaign confirm in general the excellent capability of nuclear safeguards and scientific laboratories in measuring isotopic abundances of uranium, although some problems were discovered for the measurements of the minor isotope ratios n(234U)/n(238U) and n(236U)/n(238U) and the calculation of measurement uncertainties for isotope ratios in general. This paper describes the outcome of the REIMEP 18 campaign. It includes a graphical evaluation and discussion of the results, an evaluation of the applied measurement and calibration techniques and a discussion of conclusions and actions to be taken.

  5. Variations in the uranium isotopic compositions of uranium ores from different types of uranium deposits

    NASA Astrophysics Data System (ADS)

    Uvarova, Yulia A.; Kyser, T. Kurt; Geagea, Majdi Lahd; Chipley, Don

    2014-12-01

    Variations in 238U/235U and 234U/238U ratios were measured in uranium minerals from a spectrum of uranium deposit types, as well as diagenetic phosphates in uranium-rich basins and peraluminous rhyolites and associated autunite mineralisation from Macusani Meseta, Peru. Mean δ238U values of uranium minerals relative to NBL CRM 112-A are 0.02‰ for metasomatic deposits, 0.16‰ for intrusive, 0.18‰ for calcrete, 0.18‰ for volcanic, 0.29‰ for quartz-pebble conglomerate, 0.29‰ for sandstone-hosted, 0.44‰ for unconformity-type, and 0.56‰ for vein, with a total range in δ238U values from -0.30‰ to 1.52‰. Uranium mineralisation associated with igneous systems, including low-temperature calcretes that are sourced from U-rich minerals in igneous systems, have low δ238U values of ca. 0.1‰, near those of their igneous sources, whereas uranium minerals in basin-hosted deposits have higher and more variable values. High-grade unconformity-related deposits have δ238U values around 0.2‰, whereas lower grade unconformity-type deposits in the Athabasca, Kombolgie and Otish basins have higher δ238U values. The δ234U values for most samples are around 0‰, in secular equilibrium, but some samples have δ234U values much lower or higher than 0‰ associated with addition or removal of 234U during the past 2.5 Ma. These δ238U and δ234U values suggest that there are at least two different mechanisms responsible for 238U/235U and 234U/238U variations. The 234U/238U disequilibria ratios indicate recent fluid interaction with the uranium minerals and preferential migration of 234U. Fractionation between 235U and 238U is a result of nuclear-field effects with enrichment of 238U in the reduced insoluble species (mostly UO2) and 235U in oxidised mobile species as uranyl ion, UO22+, and its complexes. Therefore, isotopic fractionation effects should be reflected in 238U/235U ratios in uranium ore minerals formed either by reduction of uranium to UO2 or chemical

  6. Uranium Isotope Systematic in Saanich Inlet

    NASA Astrophysics Data System (ADS)

    Amini, M.; Holmden, C.; Francois, R.

    2008-12-01

    As a redox-sensitive element Uranium has become the focus of stable isotope studies. Based on the nuclear field shift effect [1], U isotope fractionation was predicted as a function of U(IV)-U(VI) exchange reactions with the insoluble reduced U(IV) species being heavier than the soluble oxidized U(VI) species. Recently, variations in 238U/235U were reported in low temperature aqueous and sedimentary environments [2,3] indicating that U deposited in well-oxygenated environments is characterized by light isotopic composition, whereas suboxic and anoxic deposits tend towards a heavy isotopic signature. U isotope fractionation has been hence proposed as a promising new paleo-redox proxy. In order to test the efficacy of U isotope fractionation to record oxidation states in marine systems, we are investigating sediment samples deposited over a range of redox conditions in the seasonally anoxic Saanich Inlet, on the east coast of Vancouver Island. We have also made δ238U measurements for water samples from above and below the redoxcline. The measurements were carried out by MC-ICPMS using 233U/236U-double spike technique. The data are reported as δ238U relative to NBL 112a with a 238U/235U ratio of 137.88 (2sd). External precision is better than 0.10 permil (2sd). Eleven analyses of seawater performed over the course of this work yielded δ238U of -0.41±0.07 permil (2sd). No clear difference in δ238U values has been found, thus far, in water samples collected at 10m (O2~380μM) and 200m (O2~1μM) depths from a single location in the middle of the inlet. The mean of two measurements of the deepwater sample yielded -0.43±0.01 permil (2sd). Two measurements of the shallow water sample yielded a mean value of -0.38±0.03 permil (2sd). The δ238U values for HF-HNO3 digestions of the organic rich sediments, one taken in the middle of the basin (3.11% organic carbon) below seasonally anoxic bottom waters (-0.22±0.01 permil, n=2), and the other taken from the sill (1

  7. High precision and high accuracy isotopic measurement of uranium using lead and thorium calibration solutions by inductively coupled plasma-multiple collector-mass spectrometry

    SciTech Connect

    Bowen, I.; Walder, A.J.; Hodgson, T.; Parrish, R.R. |

    1998-12-31

    A novel method for the high accuracy and high precision measurement of uranium isotopic composition by Inductively Coupled Plasma-Multiple Collector-Mass Spectrometry is discussed. Uranium isotopic samples are spiked with either thorium or lead for use as internal calibration reference materials. This method eliminates the necessity to periodically measure uranium standards to correct for changing mass bias when samples are measured over long time periods. This technique has generated among the highest levels of analytical precision on both the major and minor isotopes of uranium. Sample throughput has also been demonstrated to exceed Thermal Ionization Mass Spectrometry by a factor of four to five.

  8. Tables for determining lead, uranium, and thorium isotope ages

    NASA Technical Reports Server (NTRS)

    Schonfeld, E.

    1974-01-01

    Tables for determining lead, uranium, and thorium isotope ages are presented in the form of computer printouts. Decay constants, analytical expressions for the functions evaluated, and the precision of the calculations are briefly discussed.

  9. Polyatomic interferences on high precision uranium isotope ratio measurements by MC-ICP-MS: Applications to environmental sampling for nuclear safeguards

    DOE PAGESBeta

    Pollington, Anthony D.; Kinman, William S.; Hanson, Susan K.; Steiner, Robert E.

    2015-09-04

    Modern mass spectrometry and separation techniques have made measurement of major uranium isotope ratios a routine task; however accurate and precise measurement of the minor uranium isotopes remains a challenge as sample size decreases. One particular challenge is the presence of isobaric interferences and their impact on the accuracy of minor isotope 234U and 236U measurements. Furthermore, we present techniques used for routine U isotopic analysis of environmental nuclear safeguards samples and evaluate polyatomic interferences that negatively impact accuracy as well as methods to mitigate their impacts.

  10. Polyatomic interferences on high precision uranium isotope ratio measurements by MC-ICP-MS: Applications to environmental sampling for nuclear safeguards

    SciTech Connect

    Pollington, Anthony D.; Kinman, William S.; Hanson, Susan K.; Steiner, Robert E.

    2015-09-04

    Modern mass spectrometry and separation techniques have made measurement of major uranium isotope ratios a routine task; however accurate and precise measurement of the minor uranium isotopes remains a challenge as sample size decreases. One particular challenge is the presence of isobaric interferences and their impact on the accuracy of minor isotope 234U and 236U measurements. Furthermore, we present techniques used for routine U isotopic analysis of environmental nuclear safeguards samples and evaluate polyatomic interferences that negatively impact accuracy as well as methods to mitigate their impacts.

  11. Isotopic evidence of natural uranium and spent fuel uranium releases into the environment.

    PubMed

    Pourcelot, L; Boulet, B; Le Corre, C; Loyen, J; Fayolle, C; Tournieux, D; Van Hecke, W; Martinez, B; Petit, J

    2011-02-01

    Uranium and plutonium isotopes were measured in soils, sediments and waters in an area subject to the past and present discharges from the uranium conversion plant of Malvési (France). The isotopes (236)U and (239)Pu are well known activation products of uranium and they prove to be powerful tracers of spent fuel releases in soils and sediments. On the other hand (234)U and (238)U activities measured in waters can be used to distinguish between releases and background uranium sources. Such findings contribute to improve the monitoring of the actinides releases by nuclear fuel facilities (mining sites, conversion, enrichment and fuel plants, reprocessing plants). PMID:21132170

  12. Uranium Isotope Ratios in Modern and Precambrian Soils

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    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.

  13. Uranium isotopes in surface waters from southern Africa

    NASA Astrophysics Data System (ADS)

    Kronfeld, J.; Vogel, J. C.

    1991-07-01

    The 234U/ 238U activity ratio in river water in southern Africa is generally higher than that reported for rivers in other regions of the world. This is interpreted as due to the prevailing environmental conditions: in this warm dry region mechanical weathering predominates over chemical weathering, causing the isotope activity ratio of leached uranium to be, on average, 2.03 ± 0.42 as compared to a ratio of 1.20 for river water in the more humid tropical and temperate regions. The isotopic composition of leachable uranium from river sediment is similar to that in the water. Rivers draining the Witwatersrand gold and uranium mining area clearly show pollution inputs characterised by high uranium content and low activity ratios.

  14. Isotopic uranium concentrations in Pullman soils of the Texas Panhandle

    SciTech Connect

    Booker, J.D.; Honea, J.H.; Gabocy, T.A.

    1995-12-31

    The study of the historic isotopic uranium data (1988 to 1994) from Pullman soils near the US Department of Energy`s Pantex Plant was undertaken to provide a range of values for native concentrations of uranium isotopes in Pullman soils of the Texas Panhandle. Offsite and onsite soil monitoring locations have been sampled since 1978. The Bushland, Texas site is used as a control location because it is upwind of the plant. Data sets for 1988 to 1993 which show significant differences from the control data set in median differences of U-234 and U-238 are summarized and discussed. Maximum uranium concentrations at Firing Sites demonstrate substantial contamination. U-234 and U-238 isotopic activity ratio results for some offsite sample locations were significantly higher than those of the control location.

  15. Origin of uranium isotope variations in early solar nebula condensates

    PubMed Central

    Tissot, François L. H.; Dauphas, Nicolas; Grossman, Lawrence

    2016-01-01

    High-temperature condensates found in meteorites display uranium isotopic variations (235U/238U), which complicate dating the solar system’s formation and whose origin remains mysterious. It is possible that these variations are due to the decay of the short-lived radionuclide 247Cm (t1/2 = 15.6 My) into 235U, but they could also be due to uranium kinetic isotopic fractionation during condensation. We report uranium isotope measurements of meteoritic refractory inclusions that reveal excesses of 235U reaching ~+6% relative to average solar system composition, which can only be due to the decay of 247Cm. This allows us to constrain the 247Cm/235U ratio at solar system formation to (1.1 ± 0.3) × 10−4. This value provides new clues on the universality of the nucleosynthetic r-process of rapid neutron capture. PMID:26973874

  16. Origin of uranium isotope variations in early solar nebula condensates.

    PubMed

    Tissot, François L H; Dauphas, Nicolas; Grossman, Lawrence

    2016-03-01

    High-temperature condensates found in meteorites display uranium isotopic variations ((235)U/(238)U), which complicate dating the solar system's formation and whose origin remains mysterious. It is possible that these variations are due to the decay of the short-lived radionuclide (247)Cm (t 1/2 = 15.6 My) into (235)U, but they could also be due to uranium kinetic isotopic fractionation during condensation. We report uranium isotope measurements of meteoritic refractory inclusions that reveal excesses of (235)U reaching ~+6% relative to average solar system composition, which can only be due to the decay of (247)Cm. This allows us to constrain the (247)Cm/(235)U ratio at solar system formation to (1.1 ± 0.3) × 10(-4). This value provides new clues on the universality of the nucleosynthetic r-process of rapid neutron capture. PMID:26973874

  17. Uranium isotope measurements by quadrupole ICP-MS for process monitoring of enrichment

    SciTech Connect

    Policke, T.A.; Bolin, R.N.; Harris, T.L.

    1998-12-31

    Historically, uranium isotopic ratio measurements in the nuclear industry have been performed using Thermal Ionization Mass Spectrometry (TIMS); primarily due to the high level of precision that can be achieved. TIMS analysis, however, requires sample purification and intricate sample loading. Quadrupole (low resolution, single detector) inductively coupled plasma--mass spectrometry, Q-ICP-MS, overcomes these disadvantages and is a cost-effective alternative, i.e., in terms of initial capital, maintenance, and operating costs. This paper presents a simple, single standard approach for measuring uranium isotope content in various solid and liquid nuclear materials along with some comparison data of Q-ICP-MS and TIMS. Intensity ratios of {sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U to total U intensity are produced, providing the enrichment level or percent {sup 235}U. A detailed description of the instrument and data collection parameters are also provided. Optimal precision and accuracy are achieved through the use of a single standard which is closely matched to the enrichment and concentration of the samples. Depending upon the standard chosen, enrichments between depleted and 97% can be quantified. Standard deviations for the major uranium isotopes are typically within 0.02 absolute and at least an order of magnitude lower for the minor U isotope abundances.

  18. Enhanced Method for Molybdenum Separation and Isotopic Determination in Geological Samples and Uranium-Rich Materials

    NASA Astrophysics Data System (ADS)

    Migeon, V.; Bourdon, B.; Pili, E.

    2014-12-01

    Molybdenum (Mo) shares analogous geochemical properties with uranium. Mo ispresent as a minor or a trace element in uranium ores under two main oxidation states: +IVand +VI. Mo has seven stable isotopes (92, 94, 95, 96, 97, 98 and 100). In natural systems,Mo and Mo isotopes were shown to fractionate during redox reactions. Because Morepresents an impurity difficult to separate in the nuclear fuel cycle, it has the potential to beused as an indicator of the origins of uranium concentrates, in the framework of nuclearforensics. This work focuses on developing an enhanced separation method for Mo from auranium-rich matrix (uranium ore, uranium concentrate) in order to analyze the massfractionation induced by processes typical of the nuclear fuel cycle. Purification of Mo forisotope ratio measurements is performed with a three-step separation on ion-exchange resins,with yields between 45 and 82%. Matrix and isobaric interferences (Zr, Ru) were reduced ingeological and uranium standards, such as U/Mo ≤ 2*10-4, Zr/Mo ≤ 1*10-3, Ru/Mo ≤ 6*10-4and Fe/Mo ≤ 4*10-3. Mo isotopic compositions were measured on a Neptune Plus MC-ICPMSequipped with Jet cones, for a concentration of 30 ng/ml. The achieved sensitivity is~1200-1800 V/ppm with interferences below 10 mV and an overall reproducibility of 0.02 ‰on the δ98Mo values. A double spike, with 97Mo and 100Mo, was added to the samples beforethe purification. It allows for correction of the chemical and instrumental mass fractionations,without requiring a quantitative yield. For igneous rocks, δ98Mo values range between -0.55and -0.03 ‰, relative to the NIST-SRM 3134 molybdenum standard. Fractionation amonguranium ore concentrates is higher, with δ98Mo ranging between 0.02 and -2.84 ‰.

  19. Evolution of isotopic composition of reprocessed uranium during the multiple recycling in light water reactors with natural uranium feed

    SciTech Connect

    Smirnov, A. Yu. Sulaberidze, G. A.; Alekseev, P. N.; Dudnikov, A. A.; Nevinitsa, V. A. Proselkov, V. N.; Chibinyaev, A. V.

    2012-12-15

    A complex approach based on the consistent modeling of neutron-physics processes and processes of cascade separation of isotopes is applied for analyzing physical problems of the multiple usage of reprocessed uranium in the fuel cycle of light water reactors. A number of scenarios of multiple recycling of reprocessed uranium in light water reactors are considered. In the process, an excess absorption of neutrons by the {sup 236}U isotope is compensated by re-enrichment in the {sup 235}U isotope. Specific consumptions of natural uranium for re-enrichment of the reprocessed uranium depending on the content of the {sup 232}U isotope are obtained.

  20. Uranium isotopes in ground water as a prospecting technique

    SciTech Connect

    Cowart, J.B.; Osmond, J.K.

    1980-02-01

    The isotopic concentrations of dissolved uranium were determined for 300 ground water samples near eight known uranium accumulations to see if new approaches to prospecting could be developed. It is concluded that a plot of /sup 234/U//sup 238/U activity ratio (A.R.) versus uranium concentration (C) can be used to identify redox fronts, to locate uranium accumulations, and to determine whether such accumulations are being augmented or depleted by contemporary aquifer/ground water conditions. In aquifers exhibiting flow-through hydrologic systems, up-dip ground water samples are characterized by high uranium concentration values (> 1 to 4 ppB) and down-dip samples by low uranium concentration values (less than 1 ppB). The boundary between these two regimes can usually be identified as a redox front on the basis of regional water chemistry and known uranium accumulations. Close proximity to uranium accumulations is usually indicated either by very high uranium concentrations in the ground water or by a combination of high concentration and high activity ratio values. Ground waters down-dip from such accumulations often exhibit low uranium concentration values but retain their high A.R. values. This serves as a regional indicator of possible uranium accumulations where conditions favor the continued augmentation of the deposit by precipitation from ground water. Where the accumulation is being dispersed and depleted by the ground water system, low A.R. values are observed. Results from the Gulf Coast District of Texas and the Wyoming districts are presented.

  1. Pulsed CO laser for isotope separation of uranium

    SciTech Connect

    Baranov, Igor Y.; Koptev, Andrey V.

    2012-07-30

    This article proposes a technical solution for using a CO laser facility for the industrial separation of uranium used in the production of fuel for nuclear power plants, employing a method of laser isotope separation of uranium with condensation repression in a free jet. The laser operation with nanosecond pulse irradiation can provide an acceptable efficiency in the separating unit and a high efficiency of the laser with the wavelength of 5.3 {mu}m. In the present work we also introduce a calculation model and define the parameters of a mode-locked CO laser with a RF discharge in the supersonic stream. The average pulsed CO laser power of 3 kW is sufficient for efficient industrial isotope separation of uranium in one stage.

  2. Uranium isotope separation from 1941 to the present

    NASA Astrophysics Data System (ADS)

    Maier-Komor, Peter

    2010-02-01

    Uranium isotope separation was the key development for the preparation of highly enriched isotopes in general and thus became the seed for target development and preparation for nuclear and applied physics. In 1941 (year of birth of the author) large-scale development for uranium isotope separation was started after the US authorities were warned that NAZI Germany had started its program for enrichment of uranium and might have confiscated all uranium and uranium mines in their sphere of influence. Within the framework of the Manhattan Projects the first electromagnetic mass separators (Calutrons) were installed and further developed for high throughput. The military aim of the Navy Department was to develop nuclear propulsion for submarines with practically unlimited range. Parallel to this the army worked on the development of the atomic bomb. Also in 1941 plutonium was discovered and the production of 239Pu was included into the atomic bomb program. 235U enrichment starting with natural uranium was performed in two steps with different techniques of mass separation in Oak Ridge. The first step was gas diffusion which was limited to low enrichment. The second step for high enrichment was performed with electromagnetic mass spectrometers (Calutrons). The theory for the much more effective enrichment with centrifugal separation was developed also during the Second World War, but technical problems e.g. development of high speed ball and needle bearings could not be solved before the end of the war. Spying accelerated the development of uranium separation in the Soviet Union, but also later in China, India, Pakistan, Iran and Iraq. In this paper, the physical and chemical procedures are outlined which lead to the success of the project. Some security aspects and Non-Proliferation measures are discussed.

  3. High-Resolution Triple Resonance Autoionization of Uranium Isotopes

    SciTech Connect

    Schumann, Philipp G.; Wendt, K; Bushaw, Bruce A.

    2005-11-01

    The near-threshold autoionization (AI) spectrum of uranium has been investigated by triple-resonance excitation with single-mode continuous lasers. Spectra were recorded over the first {approx}30 cm-1 above the first ionization limit at a resolution of 3x10-4 cm 1 using intermediate states with different J values (6, 7, 8) to assign AI level total angular momentum JAI = 5 to 9. Resonances with widths ranging from 8 MHz to 30 GHz were observed; the strongest ones have JAI = 9 and widths of {approx} 60 MHz. Hyperfine structures for 235U and isotope shifts for 234,235U have been measured in the two intermediate levels and in the final AI level for the most favorable excitation path. These measurements were performed using aqueous samples containing sub-milligram quantities of uranium at natural isotopic abundances, indicating the potential of this approach for trace isotope ratio determinations.

  4. Certification of the Uranium Isotopic Ratios in Nbl Crm 112-A, Uranium Assay Standard (Invited)

    NASA Astrophysics Data System (ADS)

    Mathew, K. J.; Mason, P.; Narayanan, U.

    2010-12-01

    Isotopic reference materials are needed to validate measurement procedures and to calibrate multi-collector ion counting detector systems. New Brunswick Laboratory (NBL) provides a suite of certified isotopic and assay standards for the US and international nuclear safeguards community. NBL Certified Reference Material (CRM) 112-A Uranium Metal Assay Standard with a consensus value of 137.88 for the 238U/235U ratio [National Bureau of Standards -- NBS, currently named National Institute for Standards and Technology, Standard Reference Material (SRM) 960 had been renamed CRM 112-A] is commonly used as a natural uranium isotopic reference material within the earth science community. We have completed the analytical work for characterizing the isotopic composition of NBL CRM 112-A Uranium Assay Standard and NBL CRM 145 (uranyl nitrate solution prepared from CRM 112-A). The 235U/238U isotopic ratios were characterized using the total evaporation (TE) and the modified total evaporation (MTE) methods. The 234U/238U isotope ratios were characterized using a conventional analysis technique and verified using the ratios measured in the MTE analytical technique. The analysis plan for the characterization work was developed such that isotopic ratios that are traceable to NBL CRM U030-A are obtained. NBL is preparing a certificate of Analysis and will issue a certificate for Uranium Assay and Isotopics. The results of the CRM 112-A certification measurements will be discussed. These results will be compared with the average values from Richter et al (2010). A comparison of the precision and accuracy of the measurement methods (TE, MTE and Conventional) employed in the certification will be presented. The uncertainties in the 235U/238U and 234U/238U ratios, calculated according to the Guide to the Expression of Uncertainty in Measurements (GUM) and the dominant contributors to the combined standard uncertainty will be discussed.

  5. Uranium isotopic composition and uranium concentration in special reference material SRM A (uranium in KCl/LiCl salt matrix)

    SciTech Connect

    Graczyk, D.G.; Essling, A.M.; Sabau, C.S.; Smith, F.P.; Bowers, D.L.; Ackerman, J.P.

    1997-07-01

    To help assure that analysis data of known quality will be produced in support of demonstration programs at the Fuel Conditioning Facility at Argonne National Laboratory-West (Idaho Falls, ID), a special reference material has been prepared and characterized. Designated SRM A, the material consists of individual units of LiCl/KCl eutectic salt containing a nominal concentration of 2.5 wt. % enriched uranium. Analyses were performed at Argonne National Laboratory-East (Argonne, IL) to determine the uniformity of the material and to establish reference values for the uranium concentration and uranium isotopic composition. Ten units from a batch of approximately 190 units were analyzed by the mass spectrometric isotope dilution technique to determine their uranium concentration. These measurements provided a mean value of 2.5058 {+-} 0.0052 wt. % U, where the uncertainty includes estimated limits to both random and systematic errors that might have affected the measurements. Evidence was found of a small, apparently random, non-uniformity in uranium content of the individual SRM A units, which exhibits a standard deviation of 0.078% of the mean uranium concentration. Isotopic analysis of the uranium from three units, by means of thermal ionization mass spectrometry with a special, internal-standard procedure, indicated that the uranium isotopy is uniform among the pellets with a composition corresponding to 0.1115 {+-} 0.0006 wt. % {sup 234}U, 19.8336 {+-} 0.0059 wt. % {sup 235}U, 0.1337 {+-} 0.0006 wt. % {sup 236}U, and 79.9171 {+-} 0.0057 wt. % {sup 238}U.

  6. Utilizing Isotopic Uranium Ratios in Groundwater Evaluations at FUSRAP Sites

    SciTech Connect

    Frederick, W.T.; Keil, K.G.; Rhodes, M.C.; Peterson, J.M.; MacDonell, M.M.

    2007-07-01

    The U.S. Army Corps of Engineers Buffalo District is evaluating environmental radioactive contamination at several Formerly Utilized Sites Remedial Action Program (FUSRAP) sites throughout New York, Pennsylvania, Ohio, and Indiana. The investigations follow the process defined in the Comprehensive Environmental Response, Compensation and Liability Act (CERCLA). Groundwater data from the Niagara Falls Storage Site (NFSS) in Lewiston, New York were evaluated for isotopic uranium ratios, specifically uranium-234 versus uranium-238 (U- 234 and U-238, respectively), and the results were presented at Waste Management 2006. Since uranium naturally occurs in all groundwater, it can be difficult to distinguish where low-concentration impacts from past releases differ from the high end of a site-specific natural background range. In natural groundwater, the ratio of U-234 to U-238 exceeds 1 (unity) due to the alpha particle recoil effect, in which U-234 is preferentially mobilized to groundwater from adjacent rock or soil. This process is very slow and may take hundreds to thousands of years before a measurable increase is seen in the natural isotopic ratio. If site releases are the source of uranium being measured in groundwater, the U-234 to U-238 ratio is commonly closer to 1, which normally reflects FUSRAP-related, uranium-contaminated wastes and soils. This lower ratio occurs because not enough residence time has elapsed since the 1940's and 1950's for the alpha particle recoil effect to have significantly altered the contamination-derived ratio. An evaluation of NFSS-specific and regional groundwater data indicate that an isotopic ratio of 1.2 has been identified as a signature value to help distinguish natural groundwater, which may have a broad background range, from zones impacted by past releases. (authors)

  7. Isotopic analysis of uranium in natural waters by alpha spectrometry

    USGS Publications Warehouse

    Edwards, K.W.

    1968-01-01

    A method is described for the determination of U234/U238 activity ratios for uranium present in natural waters. The uranium is coprecipitated from solution with aluminum phosphate, extracted into ethyl acetate, further purified by ion exchange, and finally electroplated on a titanium disc for counting. The individual isotopes are determined by measurement of the alpha-particle energy spectrum using a high resolution low-background alpha spectrometer. Overall chemical recovery of about 90 percent and a counting efficiency of 25 percent allow analyses of water samples containing as little as 0.10 ?g/l of uranium. The accuracy of the method is limited, on most samples, primarily by counting statistics.

  8. Disequilibrium of uranium isotopes in some Syrian groundwater.

    PubMed

    Abdul-Hadi, A; Alhassanieh, O; Ghafar, M

    2001-07-01

    Uranium concentration in groundwater samples from three areas of Syria was determined using alpha-spectrometry and INAA. It was in the range of 0-6.13 microg/l in the phosphate areas, and lower than 1 ppb in the volcanic areas. The activity ratio of 234U/238U was investigated, and disequilibrium of uranium isotopes was found to occur (234U/238U = 0.52-2.02). The excess of 234U was calculated. This excess can be interpreted by higher mobility of 234U, which more readily forms the soluble (UO2)2+ ion in comparison with 238U, most of which remains in the insoluble 4+ state. This excess increases with increase in uranium concentration. Thorium concentration was measured using INAA, it was found to be in the rang 0-1.15 microg/l. PMID:11339524

  9. Separation of uranium isotopes by chemical exchange

    DOEpatents

    Ogle, P.R. Jr.

    1974-02-26

    A chemical exchange method is provided for separating /sup 235/U from / sup 238/U comprising contacting a first phase containing UF/sub 6/ with a second phase containing a compound selected from the group consisting of NOUF/sub 6/, NOUF/sub 7/, and NO/sub 2/UF/sub 7/ until the U Fsub 6/ in the first phase becomes enriched in the /sup 235/U isotope. (Official Gazette)

  10. Nuclear Volume-Dependent Fractionation of Uranium Isotopes

    NASA Astrophysics Data System (ADS)

    Weyer, S.; Schauble, E. A.; Anbar, A. D.

    2007-12-01

    Chemical reactions can fractionate isotopes because the magnitudes of equilibrium and rate constants are subtly sensitive to nuclear mass. Geoscientists have exploited this fact to learn about modern environmental processes and past environmental conditions by precisely measuring variations in the isotope compositions of a wide range of elements in natural materials. Here we present evidence from natural terrestrial samples that processes related to ¡°nuclear volume¡± rather than ¡°nuclear mass¡± significantly fractionate the isotope composition of the heaviest primordial element ¨C uranium. The isotopic composition of U in nature is generally assumed to be invariant. Here, we report variations of the 238U/235U isotope ratio in natural samples (basalts, granites, seawater, corals, black shales, suboxic sediments, ferro-manganese crusts/nodules and BIFs), which span a range of δ238U values of ~ 1.3 ‰, exceeding by far the analytical precision of our method (¡Ö 0.06‰, 2SD, based on replicate measurements of individual samples). The largest isotope variations found in our survey are between oxidized and reduced depositional environments, with seawater and suboxic sediments falling in between. U isotopes were analyzed with MC-ICP-MS. A mixed 236U-233U isotopic tracer (double spike) was used to correct for isotope fractionation during sample purification and instrumental mass bias. Sediments formed in oxic environments, such as manganese crusts from the Atlantic and Pacific oceans, display δ238U of -0.54 to -0.62 ‰, slightly lighter than that of seawater (-0.41 ‰). However, sediments from reducing environments, such as black shales from the Black Sea (unit I and unit II) and the Cariaco basin, display heavy U isotope compositions with δ238U of up to +0.43 ‰ (0.84 ‰ heavier than seawater). Uranium enrichment in these sediments probably occurred during the reduction of soluble U(VI) (from seawater) to insoluble U(IV). Intriguingly, isotope

  11. Analysis on uranium isotope in the facilities of nuclear fuel materials using depleted uranium

    SciTech Connect

    Jong seon Jeon; Ki chut Jung; Sang gyu Park; Tae hyun Kim; Jae min Lee

    2007-07-01

    This study checked the degree of contamination of depleted uranium used as a chemical catalyst in the manufacturing process within the facilities of nuclear fuel materials to analyze the environmental sample for abandoning their industrial factory sites and investigated how many times of contamination were made compared to (natural) abundance of isotopes if contamination was made within the facilities. In order to analyze the degree of uranium contamination, the researcher of this study divided the upper and lower parts of 20 points from the surface of the earth within the factory site made of concrete and extracted 40 samples from the surface of the earth and 15 samples for checking air and surface water contamination. The study checked the concentration of uranium existing in small quantity in the samples by liquefying a large amount of samples using pre-treatable acid percolation. (authors)

  12. Predicting equilibrium uranium isotope fractionation in crystals and solution

    NASA Astrophysics Data System (ADS)

    Schauble, E. A.

    2015-12-01

    Despite the rapidly growing interest in using 238U/235U measurements as a proxy for changes in oxygen abundance in surface and near-surface environments, the present theoretical understanding of uranium isotope fractionation is limited to a few simple gas-phase molecules and analogues of dissolved species (e.g., 1,2,3). Understanding uranium isotope fractionation behavior in more complicated species, such as crystals and adsorption complexes, will help in the design and interpretation of experiments and field studies, and may suggest other uses for 38U/235U measurements. In this study, a recently developed first-principles method for estimating the nuclear volume component of field shift fractionation in crystals and complex molecular species (4) is combined with mass-dependent fractionation theory to predict equilibrium 38U/235U fractionations in aqueous and crystalline uranium compounds, including uraninite (UO2). The nuclear field shift effect, caused by the interaction of electrons with the finite volume of the positive charge distribution in uranium nuclei, is estimated using Density Functional Theory and the Projector Augmented Wave method (DFT-PAW). Tests against relativistic electronic structure calculations and Mössbauer isomer shift data indicate that the DFT-PAW method is reasonably accurate, while being much better suited to models of complex and crystalline species. Initial results confirm previous predictions that the nuclear volume effect overwhelms mass depdendent fractionation in U(VI)-U(IV) exchange reactions, leading to higher 238U/235U in U(IV) species (i.e., for UO2 xtal vs. UO22+aq, ln αNV ≈ +1.8‰ , ln αMD ≈ -0.8‰, ln αTotal ≈ +1.0‰ at 25ºC). UO2 and U(H2O)94+, are within ~0.4‰ of each other, while U(VI) species appear to be more variable. This suggests that speciation is likely to significantly affect natural uranium isotope fractionations, in addition to oxidation state. Tentatively, it appears that uranyl-type (UO22

  13. Uranium isotopes quantitatively determined by modified method of atomic absorption spectrophotometry

    NASA Technical Reports Server (NTRS)

    Lee, G. H.

    1967-01-01

    Hollow-cathode discharge tubes determine the quantities of uranium isotopes in a sample by using atomic absorption spectrophotometry. Dissociation of the uranium atoms allows a large number of ground state atoms to be produced, absorbing the incident radiation that is different for the two major isotopes.

  14. Uranium and strontium isotopes in Boulder Zone waters, South Florida

    SciTech Connect

    Cowart, J.B. . Dept. of Geology)

    1993-03-01

    The Boulder Zone of southern peninsular Florida, which is at a depth of approximately 1,000 m, is a cavernous, dolomitized zone which contains anomalously cool water which appears to be of marine composition. Samples of this water, as they have become available, have been analyzed for uranium concentration, U-234/U-238 alpha activity ratio, and, in a few cases, Sr-87/Sr-86 ratio and concentration. Boulder Zone samples collected in the vicinity of Ft. Lauderdale have analyzed values of the above mentioned parameters which are virtually indistinguishable from those of sea water. In a fan-like radial pattern, the uranium concentrations decrease and the U-234/U-238 activity ratios increase away from the apex at Ft. Lauderdale. It has been hypothesized by others that the Ft. Lauderdale area is the location on land that is nearest to an intake area where sea water moves into the Boulder Zone. The isotopic and concentration values reported here are consistent with this hypothesis. Waters collected from well located near the Atlantic coast north of Ft. Lauderdale do not display the same U and Sr isotopic pattern as those in the remainder of south Florida. This may be due to increased mixing between water bearing units which have been fractured and/or faulted by the extention of a flexure which has been postulated in the northern part of the study area.

  15. Utilizing Isotopic Uranium Ratios in Groundwater Evaluations at NFSS

    SciTech Connect

    Rhodes, M.C.; Keil, K.G.; Frederick, W.T.; Papura, T.R.; Leithner, J.S.; Peterson, J.M.; MacDonell, M.M.

    2006-07-01

    The U.S. Army Corps of Engineers (USACE) Buffalo District is currently evaluating environmental contamination at the Niagara Falls Storage Site (NFSS) under the Comprehensive Environmental Response, Compensation, and Liability Act (CERCLA) as part of its Formerly Utilized Sites Remedial Action Program (FUSRAP). The NFSS is located in the Town of Lewiston in western New York and has been used to store uranium-contaminated materials since 1944. Most of the radioactive materials are currently contained in an on-site structure, but past contamination remains in soil and groundwater. As a naturally occurring radionuclide, uranium is present in all groundwater. Because contamination levels at the site are quite low, it can be difficult to distinguish zones that have been impacted by the past releases from those at the high end of the natural background range. The differences in the isotopic ratio of uranium-234 (U-234) to uranium-238 (U-238) between natural groundwater systems and affected areas are being used in an innovative way to better define the nature and extent of groundwater contamination at NFSS. In natural groundwater, the ratio of U-234 to U-238 exceeds 1 due to the alpha particle recoil effect, in which U-234 is preferentially mobilized to groundwater from adjacent rock or soil. This process is very slow, and it can be hundreds to thousands of years before a measurable impact is seen in the isotopic ratio. Thus, as a result of the recoil effect, the ratio of U-234 to U-238 will be higher in natural groundwater than in contaminated groundwater. This means that if site releases were the source of the uranium being measured in groundwater at NFSS, the ratio of U-234 to U-238 would be expected to be very close to 1 (the same ratio that exists in wastes and soil at the site), because not enough time has elapsed for the alpha particle recoil effect to have significantly altered that ratio. From an evaluation of site and regional groundwater data, an isotopic ratio

  16. U-Pb isotope systematics and age of uranium mineralization, Midnite mine, Washington.

    USGS Publications Warehouse

    Ludwig, K. R.; Nash, J.T.; Naeser, C.W.

    1981-01-01

    Uranium ores at the Midnite mine, near Spokane, Washington, occur in phyllites and calcsilicates of the Proterozoic Togo Formation, near the margins of an anomalously uraniferous, porphyritic quartz monzonite of Late Cretaceous age. The present geometry of the ore zones is tabular, with the thickest zones above depressions in the pluton-country rock contact. Analyses of high-grade ores from the mine define a 207 Pb/ 204 Pb- 235 U/ 204 Pb isochron indicating an age of mineralization of 51.0 + or - 0.5 m.y. This age coincides with a time of regional volcanic activity (Sanpoil Volcanics), shallow intrusive activity, erosion, and faulting. U-Th-Pb isotopic ages of zircons from the porphyritic quartz monzonite in the mine indicate an age of about 75 m.y., hence the present orebodies were formed about 24 m.y. after its intrusion. The 51-m.y. time of mineralization probably represents a period of mobilization and redeposition of uranium by supergene ground waters, perhaps aided by mild heating and ground preparation and preserved by a capping of newly accumulated, impermeable volcanic rocks. It seems most likely that the initial concentration of uranium occurred about 75 m.y. ago, probably from relatively mild hydrothermal fluids in the contact-metamorphic aureole of the U-rich porphyritic quartz monzonite.Pitchblende, coffinitc, pyrite, marcasite, and hisingerite are the most common minerals in the uranium-bearing veinlets, with minor sphalerite and chalcopyrite. Coffinitc with associated marcasite is paragenetically later than pitchblende, though textural and isotopic evidence suggests no large difference in the times of pitchblende and colfinite formation.The U-Pb isotope systematics of total ores and of pitchblende-coffinite and pyrite-marcasite separates show that whereas open system behavior for U and Pb is essentially negligible for large (200-500 g) ore samples, Pb migration has occurred on a scale of 1 to 10 mm (out of pitchblende and coffinite and into pyrite

  17. Application of Uranium Isotope Dilution Mass Spectrometry in the preparation of New Certified Reference Materials

    NASA Astrophysics Data System (ADS)

    Hasözbek, A.; Mathew, K. J.; Orlowicz, G.; Srinivasan, B.; Narayanan, U.

    2012-04-01

    Proven measurement techniques play a critical role in the preparation of Certified Reference Materials (CRMs) - those requiring high accuracy and precision in the measurement results. Isotope Dilution Mass Spectrometry (IDMS) is one such measurement method commonly used in the quantitative analysis of uranium in nuclear safeguards and isotope geology applications. In this project, we evaluated the possibility of using some of the uranium isotopic and assay CRMs made earlier by the New Brunswick laboratory as IDMS spikes to define the uranium mass fraction in future preparations of CRMs. Uranium solutions prepared from CRM 112-A (a highly pure uranium metal assay standard) and CRM 115 (a highly pure uranium oxide isotopic and assay standard) were used as spikes in the determination of uranium. Two different thermal ionization mass spectrometer instruments (MAT 261 and TRITON) were used for the isotopic measurements. Standard IDMS equation was used for data reduction to yield results for uranium mass fraction along with uncertainties, the latter calculated according to GUM. The results show that uranium mass fraction measurements can be made with the required accuracy and precision for defining the uranium concentration in new CRMs as well as in routine samples analyses.

  18. Minor actinide transmutation in thorium and uranium matrices in heavy water moderated reactors

    SciTech Connect

    Bhatti, Zaki; Hyland, B.; Edwards, G.W.R.

    2013-07-01

    The irradiation of Th{sup 232} breeds fewer of the problematic minor actinides (Np, Am, Cm) than the irradiation of U{sup 238}. This characteristic makes thorium an attractive potential matrix for the transmutation of these minor actinides, as these species can be transmuted without the creation of new actinides as is the case with a uranium fuel matrix. Minor actinides are the main contributors to long term decay heat and radiotoxicity of spent fuel, so reducing their concentration can greatly increase the capacity of a long term deep geological repository. Mixing minor actinides with thorium, three times more common in the Earth's crust than natural uranium, has the additional advantage of improving the sustainability of the fuel cycle. In this work, lattice cell calculations have been performed to determine the results of transmuting minor actinides from light water reactor spent fuel in a thorium matrix. 15-year-cooled group-extracted transuranic elements (Np, Pu, Am, Cm) from light water reactor (LWR) spent fuel were used as the fissile component in a thorium-based fuel in a heavy water moderated reactor (HWR). The minor actinide (MA) transmutation rates, spent fuel activity, decay heat and radiotoxicity, are compared with those obtained when the MA were mixed instead with natural uranium and taken to the same burnup. Each bundle contained a central pin containing a burnable neutron absorber whose initial concentration was adjusted to have the same reactivity response (in units of the delayed neutron fraction β) for coolant voiding as standard NU fuel. (authors)

  19. Uranium Stable Isotopes: A Proxy For Productivity Or Ocean Oxygenation?

    NASA Astrophysics Data System (ADS)

    Severmann, S.

    2015-12-01

    Uranium elemental abundances in sediments have traditionally been used to reconstruct primary productivity and carbon flux in the ocean. 238U/235U isotope compositions, in contrast, are currently understood to reflect the extent of bottom water anoxia in the ocean. A review of our current understanding of authigenic U enrichment mechanism into reducing sediments suggests that a revision of this interpretation is warranted. Specifically, the current interpretation of U isotope effects in suboxic vs. anoxic deposits has not taken into account the well-documented linear relationship with organic C burial rates. Although organic C rain rates (i.e., surface productivity) and bottom water oxygenation are clearly related, distinction between these two environmental controls is conceptually important as it relates to the mechanism of enhanced C burial and ultimately the strength of the biological pump. Here we will review new and existing data to test the hypothesis that the isotope composition of authigenic U in reducing sediments are best described by their relationship with parameters related to organic carbon delivery and burial, rather than bottom water oxygen concentration.

  20. Femtosecond Laser Ablation Multicollector ICPMS Analysis of Uranium Isotopes in NIST Glass

    SciTech Connect

    Duffin, Andrew M.; Springer, Kellen WE; Ward, Jesse D.; Jarman, Kenneth D.; Robinson, John W.; Endres, Mackenzie C.; Hart, Garret L.; Gonzalez, Jhanis J.; Oropeza, Dayana; Russo, Richard; Willingham, David G.; Naes, Benjamin E.; Fahey, Albert J.; Eiden, Gregory C.

    2015-02-06

    We have utilized femtosecond laser ablation coupled to multi-collector inductively couple plasma mass spectrometry to measure the uranium isotopic content of NIST 61x (x=0,2,4,6) glasses. The uranium content of these glasses is a linear two-component mixing between isotopically natural uranium and the isotopically depleted spike used in preparing the glasses. Laser ablation results match extremely well, generally within a few ppm, with solution analysis following sample dissolution and chemical separation. In addition to isotopic data, sample utilization efficiency measurements indicate that over 1% of ablated uranium atoms reach a mass spectrometer detector, making this technique extremely efficient. Laser sampling also allows for spatial analysis and our data indicate that rare uranium concentration inhomogeneities exist in NIST 616 glass.

  1. Isotopic Analysis of Uranium in NIST SRM Glass by Femtosecond Laser Ablation

    SciTech Connect

    Duffin, Andrew M.; Hart, Garret L.; Hanlen, Richard C.; Eiden, Gregory C.

    2013-05-19

    We employed femtosecond Laser Ablation Multicollector Inductively Coupled Mass Spectrometry for the 11 determination of uranium isotope ratios in a series of standard reference material glasses (NIST 610, 612, 614, and 12 616). This uranium concentration in this series of SRM glasses is a combination of isotopically natural uranium in 13 the materials used to make the glass matrix and isotopically depleted uranium added to increase the uranium 14 elemental concentration across the series. Results for NIST 610 are in excellent agreement with literature values. 15 However, other than atom percent 235U, little information is available for the remaining glasses. We present atom 16 percent and isotope ratios for 234U, 235U, 236U, and 238U for all four glasses. Our results show deviations from the 17 certificate values for the atom percent 235U, indicating the need for further examination of the uranium isotopes in 18 NIST 610-616. Our results are fully consistent with a two isotopic component mixing between the depleted 19 uranium spike and natural uranium in the bulk glass.

  2. Determination of uranium isotopes in environmental samples by anion exchange in sulfuric and hydrochloric acid media.

    PubMed

    Popov, L

    2016-09-01

    Method for determination of uranium isotopes in various environmental samples is presented. The major advantages of the method are the low cost of the analysis, high radiochemical yields and good decontamination factors from the matrix elements, natural and man-made radionuclides. The separation and purification of uranium is attained by adsorption with strong base anion exchange resin in sulfuric and hydrochloric acid media. Uranium is electrodeposited on a stainless steel disk and measured by alpha spectrometry. The analytical method has been applied for the determination of concentrations of uranium isotopes in mineral, spring and tap waters from Bulgaria. The analytical quality was checked by analyzing reference materials. PMID:27451111

  3. Innovative lasers for uranium isotope separation. [Progress report

    SciTech Connect

    Brake, M.L.; Gilgenbach, R.M.

    1991-06-01

    Copper vapor lasers have important applications to uranium atomic vapor laser isotope separation (AVLIS). The authors have spent the first two years of their project investigating two innovative methods of exciting/pumping copper vapor lasers which have the potential to improve the efficiency and scaling of large laser systems used in uranium isotope separation. Experimental research has focused on the laser discharge kinetics of (1) microwave, and (2) electron beam excitation/pumping of large-volume copper vapor lasers. During the first year, the experiments have been designed and constructed and initial data has been taken. During the second year these experiments have been diagnosed. Highlights of some of the second year results as well as plans for the future include the following: Microwave resonant cavity produced copper vapor plasmas at 2.45 GHz, have been investigated. A CW (0--500 W) signal heats and vaporizes the copper chloride to provide the atomic copper vapor. A pulsed (5 kW, 0.5--5kHz) signal is added to the incoming CW signal via a hybrid mixer to excite the copper states to the laser levels. An enhancement of the visible radiation has been observed during the pulsed pardon of the signal. Electrical probe measurements have been implemented on the system to verify the results of the electromagnetic model formulated last year. Laser gain measurements have been initiated with the use of a commercial copper vapor laser. Measurements of the spatial profile of the emission are also currently being made. The authors plan to increase the amount of pulsed microwave power to the system by implementing a high power magnetron. A laser cavity will be designed and added to this system.

  4. Valence-associated uranium isotope fractionation of uranium enriched phosphate in a shallow aquifer, Lee County, Florida

    SciTech Connect

    Weinberg, J.M. ); Levine, B.R. ); Cowart, J.B. . Geology Dept.)

    1993-03-01

    The source of anomalously high concentrations of uranium, characterized by U-234/U-238 activity ratios significantly less than unity, in shallow groundwaters of Lee County, Florida, was investigated. Uranium in cores samples was separated into U(IV) and U(VI) oxidation state fractions, and uranium analyses were conducted by alpha spectrometry. Uranium mobility was also studied in selected leaching experiments. Results indicate that mobilization of unusually soluble uranium, present in uranium enriched phosphate of the Pliocene age Tamiami Formation at determined concentrations of up to 729 ppm, is the source for high uranium concentrations in groundwater. In leaching experiments, approximately one-third of the uranium present in the uranium enriched phosphate was mobilized into the aqueous phase. Results of previous investigations suggest that U-234, produced in rock by U-238 decay, is selectively oxidized to U(VI). The uranium enriched phosphate studied in this investigation is characterized by selective reduction of U-234, with a pattern of increasing isotopic fractionation with core depth. As a consequence, U-234/U-238 activity ratios greater than 1.0 in the U(IV) fraction, and less than 1.0 in the U(VI) fraction have developed in the rock phase. In leaching experiments, the U(VI) fraction from the rock was preferentially mobilized into the aqueous phase, suggesting that U-234/U-238 activity ratios of leaching groundwaters are strongly influenced by the isotopic characteristics of the U(VI) fraction of rock. It is suggested that preferential leaching of U(VI), present in selectivity reduced uranium enriched phosphate, is the source for low activity ratio groundwaters in Lee County.

  5. Uranium disequilibrium in groundwater: An isotope dilution approach in hydrologic investigations

    USGS Publications Warehouse

    Osmond, J.K.; Rydell, H.S.; Kaufman, M.I.

    1968-01-01

    The distribution and environmental disequilibrium patterns of naturally occurring uranium isotopes (U234 and U238) in waters of the Floridan aquifer suggest that variations in the ratios of isotopic activity and concentrations can be used quantitatively to evaluate mixing proportions of waters from differing sources. Uranium is probably unique in its potential for this approach, which seems to have general usefulness in hydrologic investigations.

  6. Uranium disequilibrium in groundwater: an isotope dilution approach in hydrologic investigations.

    PubMed

    Osmond, J K; Rydell, H S; Kaufman, M I

    1968-11-29

    The distribution and environmental disequilibrium patterns of naturally occurring uranium isotopes (U(234) and U(238)) in waters of the Floridan aquifer suggest that variations in the ratios of isotopic activity and concentrations can be used quantitatively to evaluate mixing proportions of waters from differing sources. Uranium is probably unique in its potential for this approach, which seems to have general usefulness in hydrologic investigations. PMID:4880720

  7. High-Precision Isotope Analysis of Uranium and Thorium by TIMS

    NASA Astrophysics Data System (ADS)

    Neymark, L. A.; Paces, J. B.

    2006-12-01

    The U.S. Geological Survey (USGS) Yucca Mountain Project Branch laboratory in Denver, Colorado, conducts routine high-precision isotope analyses of uranium (U) and thorium (Th) using thermal ionization mass- spectrometry (TIMS). The measurements are conducted by a ThermoFinnigan Triton\\texttrademark equipped with a Faraday multi-collector system and an energy filter in front of an active-film-type secondary electron multiplier (SEM). The abundance sensitivity of the instrument (signal at mass 237 over 238U in natural U) with the energy filter is about 15 ppb and peak tails are reduced by a factor of about 100 relative to the Faraday cup measurements. Since instrument installation in April 2004, more than 500 rock and water samples have been analyzed in support of isotope-geochemical studies for the U.S. Department of Energy`s Yucca Mountain Project. Isotope ratios of sub-nanogram to microgram U and Th samples are measured on graphite-coated single- filament and double-filament assemblies using zone-refined rhenium filaments. Ion beams less than 5 mV are measured with the SEM, which is corrected for non-linearity on the basis of measurements of NIST U-500 and 4321B standards with ion beams ranging from 0.01 to 8 mV. Inter-calibration between the SEM and the Faraday multi-collector is performed for every mass cycle using a 5 mV beam switched between Faraday cup and SEM (bridging technique), because SEM-Faraday inter-calibrations prior to the measurement failed to produce acceptable results. Either natural (^{235}U) or artificial (^{236}U, ^{229}Th) isotopes were used for the bridging. Separate runs are conducted for minor isotopes using SEM only. These techniques result in high within-run precisions of less than 0.1 to 0.2 percent for 234U/238U and 0.2 to 0.5 percent for 230Th/238U. The performance of the instrument is monitored using several U and Th isotope standards. The mean measured 234U/238U in NIST SRM 4321B is (52.879±0.004)×10-6 (95 percent confidence, n

  8. Uranium isotopic composition and absolute ages of Allende chondrules

    NASA Astrophysics Data System (ADS)

    Brennecka, G. A.; Budde, G.; Kleine, T.

    2015-11-01

    A handful of events, such as the condensation of refractory inclusions and the formation of chondrules, represent important stages in the formation and evolution of the early solar system and thus are critical to understanding its development. Compared to the refractory inclusions, chondrules appear to have a protracted period of formation that spans millions of years. As such, understanding chondrule formation requires a catalog of reliable ages, free from as many assumptions as possible. The Pb-Pb chronometer has this potential; however, because common individual chondrules have extremely low uranium contents, obtaining U-corrected Pb-Pb ages of individual chondrules is unrealistic in the vast majority of cases at this time. Thus, in order to obtain the most accurate 238U/235U ratio possible for chondrules, we separated and pooled thousands of individual chondrules from the Allende meteorite. In this work, we demonstrate that no discernible differences exist in the 238U/235U compositions between chondrule groups when separated by size and magnetic susceptibility, suggesting that no systematic U-isotope variation exists between groups of chondrules. Consequently, chondrules are likely to have a common 238U/235U ratio for any given meteorite. A weighted average of the six groups of chondrule separates from Allende results in a 238U/235U ratio of 137.786 ± 0.004 (±0.016 including propagated uncertainty on the U standard [Richter et al. 2010]). Although it is still possible that individual chondrules have significant U isotope variation within a given meteorite, this value represents our best estimate of the 238U/235U ratio for Allende chondrules and should be used for absolute dating of these objects, unless such chondrules can be measured individually.

  9. Dry Blending to Achieve Isotopic Dilution of Highly Enriched Uranium Oxide Materials

    SciTech Connect

    Henry, Roger Neil; Chipman, Nathan Alan; Rajamani, R. K.

    2001-04-01

    The end of the cold war produced large amounts of excess fissile materials in the United States and Russia. The Department of Energy has initiated numerous activities to focus on identifying material management strategies for disposition of these excess materials. To date, many of these planning strategies have included isotopic dilution of highly enriched uranium as a means of reducing the proliferation and safety risks. Isotopic dilution by dry blending highly enriched uranium with natural and/or depleted uranium has been identified as one non-aqueous method to achieve these risk (proliferation and criticality safety) reductions. This paper reviews the technology of dry blending as applied to free flowing oxide materials.

  10. Isotopic investigation of the colloidal mobility of depleted uranium in a podzolic soil.

    PubMed

    Harguindeguy, S; Crançon, P; Pointurier, F; Potin-Gautier, M; Lespes, G

    2014-05-01

    The mobility and colloidal migration of uranium were investigated in a soil where limited amounts of anthropogenic uranium (depleted in the 235U isotope) were deposited, adding to the naturally occurring uranium. The colloidal fraction was assumed to correspond to the operational fraction between 10 kDa and 1.2 μm after (ultra)filtration. Experimental leaching tests indicate that approximately 8-15% of uranium is desorbed from the soil. Significant enrichment of the leachate in the depleted uranium (DU) content indicates that uranium from recent anthropogenic DU deposit is weakly bound to soil aggregates and more mobile than geologically occurring natural uranium (NU). Moreover, 80% of uranium in leachates was located in the colloidal fractions. Nevertheless, the percentage of DU in the colloidal and dissolved fractions suggests that NU is mainly associated with the non-mobile coarser fractions of the soil. A field investigation revealed that the calculated percentages of DU in soil and groundwater samples result in the enhanced mobility of uranium downstream from the deposit area. Colloidal uranium represents between 10% and 32% of uranium in surface water and between 68% and 90% of uranium in groundwater where physicochemical parameters are similar to those of the leachates. Finally, as observed in batch leaching tests, the colloidal fractions of groundwater contain slightly less DU than the dissolved fraction, indicating that DU is primarily associated with macromolecules in dissolved fraction. PMID:24387914

  11. 77 FR 53236 - Proposed International Isotopes Fluorine Extraction Process and Depleted Uranium Deconversion...

    Federal Register 2010, 2011, 2012, 2013, 2014

    2012-08-31

    ...Notice is hereby given that the U.S. Nuclear Regulatory Commission (NRC or the Commission) has published the Final Environmental Impact Statement (EIS) for the proposed International Isotopes Fluorine Extraction Process and Depleted Uranium Deconversion Plant (INIS) in Lea County, New Mexico. On December 30, 2009, International Isotopes Fluorine Products, Inc. (IIFP), a wholly-owned subsidiary......

  12. Isotopic composition analysis and age dating of uranium samples by high resolution gamma ray spectrometry

    NASA Astrophysics Data System (ADS)

    Apostol, A. I.; Pantelica, A.; Sima, O.; Fugaru, V.

    2016-09-01

    Non-destructive methods were applied to determine the isotopic composition and the time elapsed since last chemical purification of nine uranium samples. The applied methods are based on measuring gamma and X radiations of uranium samples by high resolution low energy gamma spectrometric system with planar high purity germanium detector and low background gamma spectrometric system with coaxial high purity germanium detector. The "Multigroup γ-ray Analysis Method for Uranium" (MGAU) code was used for the precise determination of samples' isotopic composition. The age of the samples was determined from the isotopic ratio 214Bi/234U. This ratio was calculated from the analyzed spectra of each uranium sample, using relative detection efficiency. Special attention is paid to the coincidence summing corrections that have to be taken into account when performing this type of analysis. In addition, an alternative approach for the age determination using full energy peak efficiencies obtained by Monte Carlo simulations with the GESPECOR code is described.

  13. Use of uranium isotopes as a temporal and spatial tracer of nuclear contamination in the environment.

    PubMed

    Tortorello, R; Widom, E; Renwick, W H

    2013-10-01

    The Fernald Feed Materials Production Center (FFMPC) was established in 1951 to process natural uranium (U) ore, enriched uranium (EU) and depleted uranium (DU). This study tests the utility of U isotopic ratios in sediment cores and lichens as indicators of the aerial extent, degree and timing of anthropogenic U contamination, using the FFMPC as a test case. An 80-cm-long sediment core was extracted from an impoundment located approximately 6.7 km southwest of the FFMPC. Elemental concentrations of thorium (2.7-6.2 μg g(-1)) and U (0.33-1.33 μg g(-1)) as well as major and minor U isotopes were analyzed in the core. The lack of measurable (137)Cs in the deepest sample as well as a natural (235)U/(238)U signature and no measurable (236)U, are consistent with pre-FFMPC activity. Anomalously elevated U with respect to Th concentrations occur in seven consecutive samples immediately above the base of the core (62-76 cm depth). Samples with elevated U concentrations also show variable (235)U/(238)U (0.00645-0.00748), and all contain measurable (236)U ((236)U/(238)U = 2.1 × 10(-6)-3.6 × 10(-5)). Correspondence between the known releases of U dust from the FFMPC through time and variations in sediment core U concentrations, (235)U/(238)U and (236)U/(238)U ratios provide evidence for distinct releases of both DU and EU. Furthermore, these relationships demonstrate that the sediment core serves as a robust archive of past environmental U contamination events. Samples in the upper 40 cm display natural (235)U/(238)U, but measurable (236)U/(238)U ((236)U/(238)U = 5.68 × 10(-6)-1.43 × 10(-5)), further indicating the continued presence of anthropogenic U in present-day sediment. Three local lichen samples were also analyzed, and all display either EU or DU signatures coupled with elevated (236)U/(238)U, recording airborne U contamination from the FFMPC. PMID:23871969

  14. Spent fuel temperature and age determination from the analysis of uranium and plutonium isotopics

    SciTech Connect

    Scott, Mark R; Eccleston, George W; Bedell, Jeffrey J; Lockard, Chanelle M

    2009-01-01

    The capability to determine the age (time since irradiation) of spent fuel can be useful for verification and safeguards. While the age of spent fuel can be determined based on measurements of short-lived fission products, these measurements are not routinely done nor generally reported. As an alternative, age can also be determined if the uranium (U) and plutonium (Pu) isotopic values are available. Uranium isotopics are not strongly affected by fuel temperature, and bumup is determined from the {sup 235}U and {sup 236}U isotopic values. Age is calculated after estimating the {sup 241}Pu at the end of irradiation while accounting for the fuel temperature, which is determined from {sup 239}Pu or {sup 240}Pu. Burnup and age determinations are calibrated to reactor models that provide uranium and plutonium isotopics over the range of fuel irradiation. The reactor model must contain sufficient fidelity on details of the reactor type, fuel burnup, irradiation history, initial fuel enrichment and fuel temperature to obtain accurate isotopic calculations. If the latter four are unknown, they can be derived from the uranium and plutonium isotopics. Fuel temperature has a significant affect on the production of plutonium isotopics; therefore, one group cross section reactor models, such as ORIGEN, cannot be used for these calculations. Multi-group cross section set codes, such as Oak Ridge National Laboratory's TRITON code, must be used.

  15. Uranium and cadmium provoke different oxidative stress responses in Lemna minor L.

    PubMed

    Horemans, N; Van Hees, M; Van Hoeck, A; Saenen, E; De Meutter, T; Nauts, R; Blust, R; Vandenhove, H

    2015-01-01

    Common duckweed (Lemna minor L.) is ideally suited to test the impact of metals on freshwater vascular plants. Literature on cadmium (Cd) and uranium (U) oxidative responses in L. minor are sparse or, for U, non-existent. It was hypothesised that both metals impose concentration-dependent oxidative stress and growth retardation on L. minor. Using a standardised 7-day growth inhibition test, the adverse impact of these metals on L. minor growth was confirmed, with EC50 values for Cd and U of 24.1 ± 2.8 and 29.5 ± 1.9 μm, respectively, and EC10 values of 1.5 ± 0.2 and 6.5 ± 0.9 μm, respectively. The metal-induced oxidative stress response was compared through assessing the activity of different antioxidative enzymes [catalase, glutathione reductase, superoxide dismutase (SOD), ascorbate peroxidase (APOD), guaiacol peroxidase (GPOD) and syringaldizyne peroxidase (SPOD)]. Significant changes in almost all antioxidative enzymes indicated their importance in counteracting the U- and Cd-imposed oxidative burden. However, some striking differences were also observed. For activity of APODs and SODs, a biphasic but opposite response at low Cd compared to U concentrations was found. In addition, Cd (0.5-20 μm) strongly enhanced plant GPOD activity, whereas U inhibited it. Finally, in contrast to Cd, U up to 10 μm increased the level of chlorophyll a and b and carotenoids. In conclusion, although U and Cd induce similar growth arrest in L. minor, the U-induced oxidative stress responses, studied here for the first time, differ greatly from those of Cd. PMID:25073449

  16. Isotope fractionation of 238U and 235U during biologically-mediated uranium reduction

    NASA Astrophysics Data System (ADS)

    Stirling, Claudine H.; Andersen, Morten B.; Warthmann, Rolf; Halliday, Alex N.

    2015-08-01

    A series of laboratory-controlled microbial experiments using gram-negative sulphate-reducing bacteria (Desulfovibrio brasiliensis) inoculated with natural uranium were performed to investigate 238U/235U fractionation during bacterially-mediated U reduction. Control experiments, without bacteria to drive U reduction, were conducted in parallel. Paired measurements of 238U/235U and U concentration for both the residual growth medium solution and the accumulated biologically-mediated precipitate were obtained using multiple-collector inductively coupled plasma mass spectrometry (MC-ICPMS). The control experiments show that only minor (<0.1‰), if any 238U/235U fractionation occurs during co-precipitation with calcite. This implies that carbonate sediments are capable of faithfully recording the signature of the global ocean during Earth's major climatic events, including oxygenation and de-oxygenation transitions in the marine environment. The results for the microbial experiments demonstrate that the 238U/235U composition of the unreacted growth medium containing U(VI) is isotopically lighter than the composition of the U(IV)-bearing precipitate as U(VI) is consumed, in agreement with field-based observations of microbially-mediated U reduction. Uranium isotopic shifts of up to 0.8‰ were observed between the liquid and solid phases. These observations can be modelled using a Rayleigh distillation approach describing kinetic uptake in a closed system, which yields a fractionation factor α of 0.99923 ± 0.00004 (ε = -0.77 ± 04‰) for U(VI)-U(IV) reduction mediated by the D. brasiliensis microbe. This fractionation behaviour is consistent with that observed in field-based redox environments, which give rise to similar α values. Competing processes such as U co-precipitation (e.g. adsorption) may act to lower the apparent value for α and possibly play a secondary role both in the microbial experiments of this study and in natural U reduction settings where

  17. Study of uranium and thorium isotopes in ground waters and solids of two uranium mines, south Texas

    SciTech Connect

    San Juan, F.C. Jr.

    1982-01-01

    Isotopic analysis was carried out on water and solid samples taken from both the ore zones and the general vicinity of two uranium mines in south Texas. The uranium deposits were of the roll-front type. The ore-bearing formations were the Catahoula Formation of Miocene age in Duval County and the Upper Jackson formation of Eocene age in Karnes County. Solid samples were analyzed for /sup 234/U, /sup 238/U and /sup 230/Th, water for /sup 234/U and /sup 239/U. In order to test several models which have been proposed to explain the fractionation of various nuclides in the vicinity of a reduction-oxidation front, plots incorporating uranium concentration and /sup 234/U//sup 238/U activity ratio (AR) of the water and /sup 234/U//sup 238/U and /sup 230/Th//sup 238/U - /sup 234/U//sup 238/U of the solid were used. The integration of data from each of these models, including contour maps of various isotopic parameters and statistical plots helped in predicting the presence, the stage of deposition (dispersing, stable or accumulating) and the degree of radioactive disequilibrium of the deposits under study. The isotopic data were also useful in determining the position of the redox boundary and the environment of a sample. These methods may be useful in prospecting studies of other possible uranium deposits, both in the oxidized and/or the reduced environment.

  18. The minor sulfur isotope composition of Cretaceous and Cenozoic seawater sulfate

    NASA Astrophysics Data System (ADS)

    Masterson, A. L.; Wing, Boswell A.; Paytan, Adina; Farquhar, James; Johnston, David T.

    2016-06-01

    The last 125 Myr capture major changes in the chemical composition of the ocean and associated geochemical and biogeochemical cycling. The sulfur isotopic composition of seawater sulfate, as proxied in marine barite, is one of the more perplexing geochemical records through this interval. Numerous analytical and geochemical modeling approaches have targeted this record. In this study we extend the empirical isotope record of seawater sulfate to therefore include the two minor sulfur isotopes, 33S and 36S. These data record a distribution of values around means of Δ33S and Δ36S of 0.043 ± 0.016‰ and -0.39 ± 0.15‰, which regardless of δ34S-based binning strategy is consistent with a signal population of values throughout this interval. We demonstrate with simple box modeling that substantial changes in pyrite burial and evaporite sulfate weathering can be accommodated within the range of our observed isotopic values.

  19. Static, mixed-array total evaporation for improved quantitation of plutonium minor isotopes in small samples

    DOE PAGESBeta

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics “toolbox”, especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Furthermore, results are presented for small sample (~20 ng) applications involving a well-known plutoniummore » isotope reference material, CRM-126a, and compared with traditional total evaporation methods.« less

  20. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples.

    PubMed

    Stanley, F E; Byerly, Benjamin L; Thomas, Mariam R; Spencer, Khalil J

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10(-6)) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods. Graphical Abstract ᅟ. PMID:27032649

  1. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    NASA Astrophysics Data System (ADS)

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-03-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

  2. Static, Mixed-Array Total Evaporation for Improved Quantitation of Plutonium Minor Isotopes in Small Samples

    NASA Astrophysics Data System (ADS)

    Stanley, F. E.; Byerly, Benjamin L.; Thomas, Mariam R.; Spencer, Khalil J.

    2016-06-01

    Actinide isotope measurements are a critical signature capability in the modern nuclear forensics "toolbox", especially when interrogating anthropogenic constituents in real-world scenarios. Unfortunately, established methodologies, such as traditional total evaporation via thermal ionization mass spectrometry, struggle to confidently measure low abundance isotope ratios (<10-6) within already limited quantities of sample. Herein, we investigate the application of static, mixed array total evaporation techniques as a straightforward means of improving plutonium minor isotope measurements, which have been resistant to enhancement in recent years because of elevated radiologic concerns. Results are presented for small sample (~20 ng) applications involving a well-known plutonium isotope reference material, CRM-126a, and compared with traditional total evaporation methods.

  3. METHOD OF SEPARATING ISOTOPES OF URANIUM IN A CALUTRON

    DOEpatents

    Jenkins, F.A.

    1958-05-01

    Mass separation devices of the calutron type and the use of uranium hexachloride as a charge material in the calutron ion source are described. The method for using this material in a mass separator includes heating the uranium hexachloride to a temperature in the range of 60 to 100 d C in a vacuum and thereby forming a vapor of the material. The vaporized uranium hexachloride is then ionized in a vapor ionizing device for subsequent mass separation processing.

  4. Uranium and Calcium Isotope Ratio Measurements using the Modified Total Evaporation Method in TIMS

    NASA Astrophysics Data System (ADS)

    Richter, S.; Kuehn, H.; Berglund, M.; Hennessy, C.

    2010-12-01

    A new version of the "modified total evaporation" (MTE) method for isotopic analysis by multi-collector thermal ionization mass spectrometry (TIMS), with high analytical performance and designed in a more user-friendly and routinely applicable way, is described in detail. It is mainly being used for nuclear safeguards measurements of U and Pu and nuclear metrology, but can readily be applied to other scientific tasks in geochemistry, e.g. for Sr, Nd and Ca, as well. The development of the MTE method was organized in collaboration of several "key nuclear mass spectrometry laboratories", namely the New Brunswick Laboratory (NBL), the Institute for Transuranium Elements (ITU), the Safeguards Analytical Laboratory (now Safeguards Analytical Services, SGAS) of the International Atomic Energy Agency (IAEA) and the Institute for Reference Materials and Measurements (IRMM), with IRMM taking the leading role. The manufacturer of the TRITON TIMS instrument, Thermo Fisher Scientific, integrated this method into the software of the instrument. The development has now reached its goal to become a user-friendly and routinely useable method for uranium isotope ratio measurements with high precision and accuracy. Due to the use of the “total evaporation” (TE) method the measurement of the "major" uranium isotope ratio 235U/238U is routinely being performed with a precision of 0.01% to 0.02%. The use of a (certified) reference material measured under comparable conditions is emphasized to achieve an accuracy at a level of 0.02% - depending on the stated uncertainty of the certified value of the reference material. In contrast to the total evaporation method (TE), in the MTE method the total evaporation sequence is interrupted on a regular basis to allow for correction for background from peak tailing, internal calibration of a secondary electron multiplier (SEM) detector versus the Faraday cups, and ion source re-focusing. Therefore, the most significant improvement using the

  5. Neutron-rich isotope production using a uranium carbide - carbon nanotubes SPES target prototype

    NASA Astrophysics Data System (ADS)

    Corradetti, S.; Biasetto, L.; Manzolaro, M.; Scarpa, D.; Carturan, S.; Andrighetto, A.; Prete, G.; Vasquez, J.; Zanonato, P.; Colombo, P.; Jost, C. U.; Stracener, D. W.

    2013-05-01

    The SPES (Selective Production of Exotic Species) project, under development at the Istituto Nazionale di Fisica Nucleare - Laboratori Nazionali di Legnaro (INFN-LNL), is a new-generation Isotope Separation On-Line (ISOL) facility for the production of radioactive ion beams by means of the proton-induced fission of uranium. In the framework of the research on the SPES target, seven uranium carbide discs, obtained by reacting uranium oxide with graphite and carbon nanotubes, were irradiated with protons at the Holifield Radioactive Ion Beam Facility (HRIBF) of Oak Ridge National Laboratory (ORNL). In the following, the yields of several fission products obtained during the experiment are presented and discussed. The experimental results are then compared to those obtained using a standard uranium carbide target. The reported data highlights the capability of the new type of SPES target to produce and release isotopes of interest for the nuclear physics community.

  6. The jackknife as an approach for uncertainty assessment in gamma spectrometric measurements of uranium isotope ratios

    NASA Astrophysics Data System (ADS)

    Ramebäck, H.; Vesterlund, A.; Tovedal, A.; Nygren, U.; Wallberg, L.; Holm, E.; Ekberg, C.; Skarnemark, G.

    2010-08-01

    The jackknife as an approach for uncertainty estimation in gamma spectrometric uranium isotope ratio measurements was evaluated. Five different materials ranging from depleted uranium (DU) to high enriched uranium (HEU) were measured using gamma spectrometry. High resolution inductively coupled plasma mass spectrometry (ICP-SFMS) was used as a reference method for comparing the results obtained with the gamma spectrometric method. The relative combined uncertainty in the gamma spectrometric measurements of the 238U/ 235U isotope ratio using the jackknife was about 10-20% ( k = 2), which proved to be fit-for-purpose in order to distinguish between different uranium categories. Moreover, the enrichment of 235U in HEU could be measured with an uncertainty of 1-2%.

  7. Laser ablation inductively coupled plasma mass spectrometry measurement of isotope ratios in depleted uranium contaminated soils.

    PubMed

    Seltzer, Michael D

    2003-09-01

    Laser ablation of pressed soil pellets was examined as a means of direct sample introduction to enable inductively coupled plasma mass spectrometry (ICP-MS) screening of soils for residual depleted uranium (DU) contamination. Differentiation between depleted uranium, an anthropogenic contaminant, and naturally occurring uranium was accomplished on the basis of measured 235U/238U isotope ratios. The amount of sample preparation required for laser ablation is considerably less than that typically required for aqueous sample introduction. The amount of hazardous laboratory waste generated is diminished accordingly. During the present investigation, 235U/238U isotope ratios measured for field samples were in good agreement with those derived from gamma spectrometry measurements. However, substantial compensation was required to mitigate the effects of impaired pulse counting attributed to sample inhomogeneity and sporadic introduction of uranium analyte into the plasma. PMID:14611049

  8. Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain).

    PubMed

    Camacho, A; Devesa, R; Vallés, I; Serrano, I; Soler, J; Blázquez, S; Ortega, X; Matia, L

    2010-12-01

    A study is presented on the distribution of (234)U, (238)U, (235)U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261mBqL(-1). The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The (234)U/(238)U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of (234)U/(238)U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found. PMID:20870317

  9. Rapid determination of uranium isotopes in urine by inductively coupled plasma-mass spectrometry.

    PubMed

    Shi, Y; Dai, X; Collins, R; Kramer-Tremblay, S

    2011-08-01

    Following a radiological or nuclear emergency involving uranium exposure, rapid analytical methods are needed to analyze the concentration of uranium isotopes in human urine samples for early dose assessment. The inductively coupled plasma mass spectrometry (ICP-MS) technique, with its high sample throughput and high sensitivity, has advantages over alpha spectrometry for uranium urinalysis after minimum sample preparation. In this work, a rapid sample preparation method using an anion exchange chromatographic column was developed to separate uranium from the urine matrix. A high-resolution sector field ICP-MS instrument, coupled with a high sensitivity desolvation sample introduction inlet, was used to determine uranium isotopes in the samples. The method can analyze up to 24 urine samples in two hours with the limits of detection of 0.0014, 0.10, and 2.0 pg mL(-1) for (234)U, (235)U, and (238)U, respectively, which meet the requirement for isotopic analysis of uranium in a radiation emergency. PMID:21709502

  10. Uranium Isotopic and Quantitative Analysis Using a Mechanically-Cooled HPGe Detector

    SciTech Connect

    Solodov, Alexander A

    2008-01-01

    A new, portable high-resolution spectroscopy system based on a high-purity germanium detector cooled with a miniature Stirling-cycle cooler, ORTEC trans-SPEC, has recently become commercially available. The use of a long-life mechanical cooling system eliminates the need for liquid nitrogen. The purpose of this study was to determine the applicability of this new instrument for isotopic and quantitative analyses of uranium samples. The results of the performance of the trans-SPEC with the combination of PC-FRAM and ISOTOPIC software packages are described in this paper. An optimal set of analysis parameters for uranium measurements is proposed.

  11. Method and apparatus for storing hydrogen isotopes. [stored as uranium hydride in a block of copper

    DOEpatents

    McMullen, J.W.; Wheeler, M.G.; Cullingford, H.S.; Sherman, R.H.

    1982-08-10

    An improved method and apparatus for storing isotopes of hydrogen (especially tritium) are provided. The hydrogen gas is stored as hydrides of material (for example uranium) within boreholes in a block of copper. The mass of the block is critically important to the operation, as is the selection of copper, because no cooling pipes are used. Because no cooling pipes are used, there can be no failure due to cooling pipes. And because copper is used instead of stainless steel, a significantly higher temperature can be reached before the eutectic formation of uranium with copper occurs, (the eutectic of uranium with the iron in stainless steel forms at a significantly lower temperature).

  12. Simultaneous determination of the quantity and isotopic ratios of uranium in individual micro-particles by isotope dilution thermal ionization mass spectrometry (ID-TIMS).

    PubMed

    Park, Jong-Ho; Choi, Eun-Ju

    2016-11-01

    A method to determine the quantity and isotopic ratios of uranium in individual micro-particles simultaneously by isotope dilution thermal ionization mass spectrometry (ID-TIMS) has been developed. This method consists of sequential sample and spike loading, ID-TIMS for isotopic measurement, and application of a series of mathematical procedures to remove the contribution of uranium in the spike. The homogeneity of evaporation and ionization of uranium content was confirmed by the consistent ratio of n((233)U)/n((238)U) determined by TIMS measurements. Verification of the method was performed using U030 solution droplets and U030 particles. Good agreements of resulting uranium quantity, n((235)U)/n((238)U), and n((236)U)/n((238)U) with the estimated or certified values showed the validity of this newly developed method for particle analysis when simultaneous determination of the quantity and isotopic ratios of uranium is required. PMID:27591656

  13. Uranium Measurement Improvements at the Savannah River Technology Center

    SciTech Connect

    Shick, C. Jr.

    2002-02-13

    Uranium isotope ratio and isotope dilution methods by mass spectrometry are used to achieve sensitivity, precision and accuracy for various applications. This report presents recent progress made at SRTC in the analysis of minor isotopes of uranium. Comparison of routine measurements of NBL certified uranium (U005a) using the SRTC Three Stage Mass Spectrometer (3SMS) and the SRTC Single Stage Mass Spectrometer (SSMS). As expected, the three stage mass spectrometer yielded superior sensitivity, precision, and accuracy for this application.

  14. Syndepositional diagenesis of modern platform carbonates: Evidence from isotopic and minor element data

    NASA Astrophysics Data System (ADS)

    Patterson, William P.; Walter, Lynn M.

    1994-02-01

    Physical, elemental, and stable isotopic evidence documents significant syndepositional diagenesis off biogenic carbonate in modern sediment pore water. Halimeda (aragonite) and Neogoniolithon (high-Mg calcite) fragments from sediment cores and experimental substrates were compared with fresh samples to determine the magnitude of minor element (Sr, Mg), and stable isotopic (C and O) compositional shifts. Although no significant shift in bulk sediment mineralogy is apparent, experimental substrates and natural biogenic grains exhibit significant diagenetic changes. These changes include dissolution textures, net loss of mass, changes in minor element composition, and progressive evolution toward carbon and oxygen isotopic equilibrium with p ore water. Our results demonstrate that carbonate sediment can undergo rapid syndepositional dissolution and reprecipitation. Pore waters likely are buffered chemically and isotopically by most abundant carbonate grain types. In turn, compositions of less abundant carbonate grains may shift toward equilibrium with respect to pore water. Therefore, many components of shelf limestone have compositions controlled by chemically evolved pore waters rather than by seawater from which the biotic carbonate originally precipitated.

  15. Graphite Isotope Ratio Method Development Report: Irradiation Test Demonstration of Uranium as a Low Fluence Indicator

    SciTech Connect

    Reid, B.D.; Gerlach, D.C.; Love, E.F.; McNeece, J.P.; Livingston, J.V.; Greenwood, L.R.; Petersen, S.L.; Morgan, W.C.

    1999-10-20

    This report describes an irradiation test designed to investigate the suitability of uranium as a graphite isotope ratio method (GIRM) low fluence indicator. GIRM is a demonstrated concept that gives a graphite-moderated reactor's lifetime production based on measuring changes in the isotopic ratio of elements known to exist in trace quantities within reactor-grade graphite. Appendix I of this report provides a tutorial on the GIRM concept.

  16. Isotope ratios of uranium using high resolution inductively coupled plasma-mass spectrometry (ICP-MS)

    SciTech Connect

    Hearn, R.; Wildner, H.

    1998-12-31

    Actinide element isotope ratios have been determined in environmental samples using high resolution ICP-MS with ultrasonic nebulization. Precisions as low as 0.1% RSD have been achieved using various methods of acquisition. The methodology has been used for environmental monitoring of uranium isotope ratios as an indicator of nuclear activity. Also, it has been applied to calcite dating studies as a measure of past geochemical disturbances.

  17. Isotopes of uranium and plutonium in the atmosphere. [Cosmos-954 fall in Canada

    SciTech Connect

    Sakuragi, Y.

    1982-01-01

    The activities of /sup 234/U, /sup 235/U and /sup 238/U were measured in 24 individual rain samples and two composite rains collected at Fayetteville, Arkansas, during the months of March 1979 and March 1980 through May 1981. Uranium-234 and -235 were found to be highly enriched in several rain samples collected during the months of April and May 1980. Uranium-238 concentrations, on the other hand, were unusually high during the months of July, August and early September 1980. The concentrations of /sup 238/Pu and /sup 238/ /sup 240/Pu were measured in 76 individual rain samples and two composite rains which were collected at Fayetteville, Arkansas, during the period from February 1979 through December 1980. Plutonium-238 and plutonium-239,240 concentrations were found to be extremely high during the months of July, August and early September 1980. The anomalous uranium highly enriched in the light isotopes of uranium appears to have originated from the Soviet satellite Cosmos-954 which fell over Canada on 24 January 1978. The uranium fallout occurred just about the time Mount St. Helens erupted on 18 May 1980 and began to inject a large amount of natural uranium into the atmosphere. The pattern of variations of the concentrations of /sup 238/U in rain after the eruption of Mount St. Helens was found to be similar to that of plutonium isotopes.

  18. Spatial heterogeneity of uranium isotope variations in a Phanerozoic, epicontintental black shale (Hushpuckney Shale, Swope Formation)

    NASA Astrophysics Data System (ADS)

    Herrmann, A. D.; Gordon, G. W.; Romaniello, S. J.; Algeo, T. J.; Anbar, A. D.

    2012-12-01

    It has recently been shown that substantial variations in the 238U/235U ratio exist in nature. The isotopic composition of seawater is ultimately driven by the relative sizes and isotopic signatures of the major sources and sinks. Rivers are the major sources of uranium to the ocean, and reducing sediments (mainly anoxic and suboxic sediments) are the major sinks. Under reducing conditions heavy uranium isotopes are sequestered preferentially. Because of the long residence time of uranium in the global ocean, and the relatively large fractionation during removal of uranium under reducing conditions, it has been suggested that the isotope composition of seawater might reflect changes in the redox state of the ocean and that such changes might be mirrored in black shales. Here we present uranium isotope variations of a Pennsylvanian black shale (Hushpuckney Shale; Swope Formation) from two cores from the same depositional basin (Late Paleozoic Midcontinent Sea; LPMS) to test whether global marine redox conditions can be determined from a single section in epicontinental settings. If uranium isotopes in epicontinental black shales can be used to quantify changes in redox changes of the global ocean, then contemporaneous black shales sections should have the same isotope trends and magnitudes. The Hushpuckney shale is one of several cyclothem core intervals that were deposited over large areas (tens of thousands of square kilometers) on continental crust during early transgression in response to the deglaciation of large icesheets in the southern hemisphere. The two cores investigated for this study represent a transect through the LPMS from close to the open ocean (SE Kansas) towards the shoreline (Iowa). The Hushpuckney shale can be easily identified and correlated in these two cores. Thus, it offers an excellent opportunity to test whether the uranium isotopic composition is similar across the basin and how much local redox conditions can play a role in faithfully

  19. Status of Uranium Atomic Vapor Laser Isotope Separation Program

    SciTech Connect

    Chen, Hao-Lin; Feinberg, R.M.

    1993-06-01

    This report discusses demonstrations of plant-scale hardware embodying AVLIS technology which were completed in 1992. These demonstrations, designed to provide key economic and technical bases for plant deployment, produced significant quantities of low enriched uranium which could be used for civilian power reactor fuel. We are working with industry to address the integration of AVLIS into the fuel cycle. To prepare for deployment, a conceptual design and cost estimate for a uranium enrichment plant were also completed. The U-AVLIS technology is ready for commercialization.

  20. Investigation of the Photochemical Method for Uranium Isotope Separation

    DOE R&D Accomplishments Database

    Urey, H. C.

    1943-07-10

    To find a process for successful photochemical separation of isotopes several conditions have to be fulfilled. First, the different isotopes have to show some differences in the spectrum. Secondly, and equally important, this difference must be capable of being exploited in a photochemical process. Parts A and B outline the physical and chemical conditions, and the extent to which one might expect to find them fulfilled. Part C deals with the applicability of the process.

  1. Uranium isotope fractionation during coprecipitation with aragonite and calcite

    NASA Astrophysics Data System (ADS)

    Chen, Xinming; Romaniello, Stephen J.; Herrmann, Achim D.; Wasylenki, Laura E.; Anbar, Ariel D.

    2016-09-01

    Natural variations in 238U/235U of marine calcium carbonates might provide a useful way of constraining redox conditions of ancient environments. In order to evaluate the reliability of this proxy, we conducted aragonite and calcite coprecipitation experiments at pH ∼7.5 and ∼8.5 to study possible U isotope fractionation during incorporation into these minerals. Small but significant U isotope fractionation was observed in aragonite experiments at pH ∼8.5, with heavier U isotopes preferentially enriched in the solid phase. 238U/235U of dissolved U in these experiments can be fit by Rayleigh fractionation curves with fractionation factors of 1.00007 + 0.00002/-0.00003, 1.00005 ± 0.00001, and 1.00003 ± 0.00001. In contrast, no resolvable U isotope fractionation was observed in an aragonite experiment at pH ∼7.5 or in calcite experiments at either pH. Equilibrium isotope fractionation among different aqueous U species is the most likely explanation for these findings. Certain charged U species are preferentially incorporated into calcium carbonate relative to the uncharged U species Ca2UO2(CO3)3(aq), which we hypothesize has a lighter equilibrium U isotope composition than most of the charged species. According to this hypothesis, the magnitude of U isotope fractionation should scale with the fraction of dissolved U that is present as Ca2UO2(CO3)3(aq). This expectation is confirmed by equilibrium speciation modeling of our experiments. Theoretical calculation of the U isotope fractionation factors between different U species could further test this hypothesis and our proposed fractionation mechanism. These findings suggest that U isotope variations in ancient carbonates could be controlled by changes in the aqueous speciation of seawater U, particularly changes in seawater pH, PCO2 , Ca2+, or Mg2+ concentrations. In general, these effects are likely to be small (<0.13‰), but are nevertheless potentially significant because of the small natural range of

  2. A method for the rapid radiochemical analysis of uranium and thorium isotopes in impure carbonates.

    PubMed

    Elyahyaoui, A; Zarki, R; Chiadli, A

    2003-01-01

    A simple method combining solvent extraction and electrodeposition procedures is described for the determination of the isotopic composition and content of uranium and thorium in travertine samples. The actinide elements are extracted with diethyl ether from a calcium nitrate solution. The isolation of the elements and the alpha source preparation are performed in two steps after the sample digestion. The acid leaching of samples is performed using both partial and total dissolution methods. High recoveries of both uranium and thorium and good alpha-spectra are obtained with both partial and total dissolution methods. PMID:12485673

  3. Influence of nutrient medium composition on uranium toxicity and choice of the most sensitive growth related endpoint in Lemna minor.

    PubMed

    Horemans, Nele; Van Hees, May; Saenen, Eline; Van Hoeck, Arne; Smolders, Valérie; Blust, Ronny; Vandenhove, Hildegarde

    2016-01-01

    Uranium (U) toxicity is known to be highly dependent on U speciation and bioavailability. To assess the impact of uranium on plants, a growth inhibition test was set up in the freshwater macrophyte Lemna minor. First growth media with different compositions were tested in order to find a medium fit for testing U toxicity in L. minor. Following arguments were used for medium selection: the ability to sustain L. minor growth, a high solubility of U in the medium and a high percentage of the more toxic U-species namely UO2(2+). Based on these selection criteria a with a low phosphate concentration of 0.5 mg L(-1) and supplemented with 5 mM MES (2-(N-morpholino)ethanesulfonic acid) to ensure pH stability was chosen. This medium also showed highest U toxicity compared to the other tested media. Subsequently a full dose response curve for U was established by exposing L. minor plants to U concentrations ranging from 0.05 μM up to 150 μM for 7 days. Uranium was shown to adversely affect growth of L. minor in a dose dependent manner with EC10, EC30 and EC50 values ranging between 1.6 and 4.8 μM, 7.7-16.4 μM and 19.4-37.2 μM U, respectively, depending on the growth endpoint. Four different growth related endpoints were tested: frond area, frond number, fresh weight and dry weight. Although differences in relative growth rates and associated ECx-values calculated on different endpoints are small (maximal twofold difference), frond area is recommended to be used to measure U-induced growth effects as it is a sensitive growth endpoint and easy to measure in vivo allowing for measurements over time. PMID:26187266

  4. Analysis of Concentrated Uranium Ores Using Stable Isotopes and Elemental Concentrations

    NASA Astrophysics Data System (ADS)

    Miller, D. L.; Riciputi, L. R.; Buerger, S.; Horita, J.; Bostick, D.

    2006-12-01

    The illicit trafficking of nuclear materials presents a continuing threat to national and international security. Various geochemical characteristics of yellowcake (concentrated uranium ore) could potentially provide information on the geologic, geographic, and processing origin of the ore. We have been focusing on investigating the potential of stable isotope analyses, namely carbon, nitrogen, and oxygen, to provide "forensic" information about ore environment and artificial processing methods used to concentrate the uranium ore. Stable isotope analysis of carbon and nitrogen was performed using a Costech elemental analyzer (EA) attached to a Finnigan Mat 252 mass spectrometer. Carbon and nitrogen isotopes can be characteristic of the processing agents used to concentrate the uranium ore. Oxygen analysis was performed using a ThermoFinnigan thermal conversion elemental analyzer (TCEA) attached to a Finnigan Mat 252 mass spectrometer at ORNL. In addition to the stable isotope analyses, elemental concentrations were analyzed using time-of-flight ICP-MS, and uranium isotope composition measured using MC-ICP-MS. Results from a number of yellowcake samples will be presented, illustrating the potential of geochemical characteristics to distinguish among different types of samples. Research sponsored by the Office of Nonproliferation and International Security (NA-24), National Nuclear Security Administration (NNSA), U.S. Department of Energy, under contract DE-AC05-00OR22725 with Oak Ridge National Laboratory, managed and operated by UT-Battelle, LLC. The submitted manuscript has been authored by a contractor of the U.S. Government under contract No. DE- AC05-00OR22725. Accordingly, the U.S. Government retains a nonexclusive, royalty-free license to publish or reproduce the published form of this contribution, or allow others to do so, for U.S. Government purposes.

  5. MEASUREMENTS OF RADON, THORON, ISOTOPIC URANIUM AND THORIUM TO DETERMINE OCCUPATIONAL & ENVIRONMENTAL EXPOSURE & RISK AT FERNALD FEED MATERIALS PRODUCTION CENTER.

    EPA Science Inventory

    The research at the Fernald Environmental Restoration Management Corporation (FERMCO) site will provide radionuclide data, and realistic risk evaluation for isotopic radon, thorium, uranium and lead exposure.We have developed and tested a passive radon monitor with proven accur...

  6. Uranium Isotopic Fractionation Induced by U(VI) Adsorption Onto Common Aquifer Minerals

    NASA Astrophysics Data System (ADS)

    Jemison, N.; Johnson, T. M.; Shiel, A. E.; Lundstrom, C.

    2014-12-01

    Mining and processing of uranium (U) ore for nuclear energy and weapons has led to U contamination of groundwater. Reduction of soluble, mobile U(VI) to UO2 decreases uranium groundwater concentrations and is an important driver of natural and stimulated attenuation. 238U/235U measurements can be used to monitor and perhaps quantify U(VI) reduction; biological reduction of U(VI) has been shown to produce a ~1.0‰ isotopic fractionation in both laboratory and field settings, with the reduced product enriched in 238U. However, adsorption of U(VI) onto minerals may complicate the use of 238U/235U in this application; adsorption of U(VI) onto Mn oxides induces an isotopic fractionation of 0.2‰ with the sorbed U(VI) depleted in 238U. At present, the isotopic shift produced by adsorption of U(VI) onto other minerals has not yet been explored. This study measures U isotopic fractionation during adsorption onto goethite, birnessite, quartz, illite, and complex aquifer materials. In addition, the effect of U speciation on fractionation is also examined by adsorption of uranyl (UO22+), uranyl carbonato (such as UO2(CO3)22- and UO2(CO3)34-), and calcium uranyl carbonato (Ca2UO2(CO3)3(aq) and CaUO2(CO3)32-) ions to goethite and birnessite. Experiments are carried out with a multi-stage, batch approach, in which a U(VI)-bearing solution is exposed to three stages of adsorption, and the final solution is analyzed by a double-spike MC-ICP-MS method. This increases our ability to resolve among sorbents the extent of fractionation. Early results suggest that uranium adsorption to different minerals produces different isotopic fractionations, with quartz producing little to no fractionation (<0 .05‰), while goethite produces a 0.16‰ isotopic shift (adsorbed U(VI) depleted in 238U).

  7. Theoretical investigations of uranium isotope fractionation caused by nuclear volume effects

    NASA Astrophysics Data System (ADS)

    Yang, S.

    2015-12-01

    Because the half-life times of uranium isotopes are all very long, e.g., 4.5Ga for 238U and 0.7Ga for 235U, people actually treat uranium isotope system as a stable one in many young geologic systems (e.g., Bopp et al., 2010; Basu et al., 2014). There is an increasing trend of using U isotope method to study surface geochemistry problems. For example, people start to use U isotopes as a new tracer to determine the change of redox conditions (Holmden et al., 2015; Wang et al., 2015). However, there are only a few equilibrium U isotope fractionation factors available right now. The new enterprise of U isotope method requires a much expanded data-base of equilibrium U isotope fractionation factor. Many evidences showed that heavy isotope systems could be significantly fractionated as the consequence of the nuclear volume effect (NVE) or so-called nuclear field shift effect,which is a driving force of mass-independent fractionation induced by differences in nuclear size and nuclear shape of isotopes. Here we theoretically estimate the magnitude of equilibrium isotope fractionation factors of U-bearing gaseous and solid compounds caused by NVE via density functional theory (DFT) quantum chemistry methods with careful evaluation on quantum relativistic effects. Our calculation results show the NVE drives 238U/235U fractionations can be up to -4.43‰ between U(VI) and U(IV) species, or can be up to -1.68‰ between U(IV) and U(III) species, at room temperature. The U4+-bearing species or phases tend to enrich heavier isotopes (i.e., 238U) relative to the oxidized phases (U6+-bearing), and enrich lighter isotopes (i.e., 235U) relative to the reduced U(III) phases (U3+-bearing), which generally agree with the recent experimental results (Wang et al., 2015). Our results provide a base for broad applications of equilibrium U isotope fractionation in surface environments.

  8. The Schwartzwalder uranium deposit, II: Age of uranium mineralization and lead isotope constraints on genesis.

    USGS Publications Warehouse

    Ludwig, K. R.; Wallace, A.R.; Simmons, K.R.

    1985-01-01

    Schwartzwalder ores have high amounts of initial (common) Pb that was both variable and relatively radiogenic in its isotope ratios. Assuming the common Pb in these ores to have sources of similar age and similar Th/U, samples with initial Pb isotope ratios are identified - and others with variable initial ratios are normalized - to obtain U-Pb isochrons yielding an early Laramide age of 69.3 + or - 1.1 m.y. for the ores. The initial Pb-isotope systematics indicate local sources of U, dispersed in concentrations <100 ppm, in rocks of 1730 + or - 130 m.y. age. -G.J.N.

  9. Uranium isotopic ratio measurements of U3O8 reference materials by atom probe tomography.

    PubMed

    Fahey, Albert J; Perea, Daniel E; Bartrand, Jonah; Arey, Bruce W; Thevuthasan, Suntharampillai

    2016-03-01

    We report results of measurements of isotopic ratios obtained with atom probe tomography on U3O8 reference materials certified for their isotopic abundances of uranium. The results show good agreement with the certified values. High backgrounds due to tails from adjacent peaks complicate the measurement of the integrated peak areas as well as the fact that only oxides of uranium appear in the spectrum, the most intense of which is doubly charged. In addition, lack of knowledge of other instrumental parameters, such as the dead time, may bias the results. Isotopic ratio measurements can be performed at the nanometer-scale with the expectation of sensible results. The abundance sensitivity and mass resolving power of the mass spectrometer are not sufficient to compete with magnetic-sector instruments but are not far from measurements made by ToF-SIMS of other isotopic systems. The agreement of the major isotope ratios is more than sufficient to distinguish most anthropogenic compositions from natural. PMID:26774651

  10. Uranium Isotopic Ratio Measurements of U3O8 Reference Materials by Atom Probe Tomography

    SciTech Connect

    Fahey, Albert J.; Perea, Daniel E.; Bartrand, Jonah AG; Arey, Bruce W.; Thevuthasan, Suntharampillai

    2016-01-01

    We report results of measurements of isotopic ratios obtained with atom probe tomography on U3O8 reference materials certified for their isotopic abundances of uranium. The results show good agreement with the certified values. High backgrounds due to tails from adjacent peaks complicate the measurement of the integrated peak areas as well as the fact that only oxides of uranium appear in the spectrum, the most intense of which is doubly charged. In addition, lack of knowledge of other instrumental parameters, such as the dead time, may bias the results. Isotopic ratio measurements can be performed at the nanometer-scale with the expectation of sensible results. The abundance sensitivity and mass resolving power of the mass spectrometer are not sufficient to compete with magnetic-sector instruments but are not far from measurements made by ToF-SIMS of other isotopic systems. The agreement of the major isotope ratios is more than sufficient to distinguish most anthropogenic compositions from natural.

  11. Improving precision in resonance ionization mass spectrometry : influence of laser bandwidth in uranium isotope ratio measurements.

    SciTech Connect

    Isselhardt, B. H.; Savina, M. R.; Knight, K. B.; Pellin, M. J.; Hutcheon, I. D.; Prussin, S. G.

    2011-03-01

    The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of {sup 235}U/{sup 238}U ratios by resonance ionization mass spectrometry (RIMS) to decrease laser-induced isotopic fractionation. By broadening the bandwidth of the first laser in a three-color, three-photon ionization process from a bandwidth of 1.8 GHz to about 10 GHz, the variation in sequential relative isotope abundance measurements decreased from 10% to less than 0.5%. This procedure was demonstrated for the direct interrogation of uranium oxide targets with essentially no sample preparation.

  12. A new series of uranium isotope reference materials for investigating the linearity of secondary electron multipliers in isotope mass spectrometry

    NASA Astrophysics Data System (ADS)

    Richter, S.; Alonso, A.; Aregbe, Y.; Eykens, R.; Kehoe, F.; Kühn, He; Kivel, N.; Verbruggen, A.; Wellum, R.; Taylor, P. D. P.

    2009-04-01

    A new series of gravimetrically prepared uranium isotope reference materials, the so-called IRMM-074 series, with the n(235U)/n(238U) isotope ratio held constant at unity and the n(233U)/n(238U) isotope ratios varying from 1.0 to 10-6 has been prepared and certified. This series is suited for calibration of secondary electron multipliers used widely in isotope mass spectrometry, in particular for techniques such as thermal ionization mass spectrometry (TIMS), inductively coupled plasma mass spectrometry (ICPMS), accelerator mass spectrometry (AMS) and resonance ionization mass spectrometry (RIMS). The new IRMM-074 was prepared as a replacement for the already exhausted IRMM-072 predecessor series. Uranium materials with high isotopic enrichments of 233U, 235U and 238U were purified using identical methods involving separation on anion and cation column followed by a precipitation as peroxide. The oxides were calcined to convert them to U3O8 simultaneously, in an oven installed in a glove-box that provided a controlled low-humidity environment. The oxides of 235U and 238U were weighed and mixed with a mole ratio n(235U)/n(238U) = 1.0 and then dissolved. The 233U oxide was dissolved to form a separate solution with the same concentration and 6rom this primary solution three dilutions were made by weighing. A weighed amount of the n(235U)/n(238U) solution and weighed amounts of the 233U solutions were mixed in various proportions in order to achieve n(233U)/n(238U) isotope ratios varying from 1.0 to 10-6. The methods for the preparation, the mixing and the mixing calculations are described. The expanded uncertainties (coverage factor k = 2) of the certified isotope ratios for the IRMM-074 series are 0.015% for the n(235U)/n(238U) ratio and 0.025% for the n(233U)/n(238U) ratios, which constitutes an improvement compared to those of the predecessor IRMM-072 series. In addition, recent observations regarding the linearity response of secondary electron multipliers (SEMs

  13. Trace elements and Pb isotopes in soils and sediments impacted by uranium mining.

    PubMed

    Cuvier, A; Pourcelot, L; Probst, A; Prunier, J; Le Roux, G

    2016-10-01

    The purpose of this study is to evaluate the contamination in As, Ba, Co, Cu, Mn, Ni, Sr, V, Zn and REE, in a high uranium activity (up to 21,000Bq∙kg(-1)) area, downstream of a former uranium mine. Different geochemical proxies like enrichment factor and fractions from a sequential extraction procedure are used to evaluate the level of contamination, the mobility and the availability of the potential contaminants. Pb isotope ratios are determined in the total samples and in the sequential leachates to identify the sources of the contaminants and to determine the mobility of radiogenic Pb in the context of uranium mining. In spite of the large uranium contamination measured in the soils and the sediments (EF≫40), trace element contamination is low to moderate (2isotopic signature of the contaminated soils is strongly radiogenic. Measurements performed on the sequential leachates reveal inputs of radiogenic Pb in the most mobile fractions of the contaminated soil. Inputs of low-mobile radiogenic Pb from mining activities may also contribute to the Pb signature recorded in the residual phase of the contaminated samples. We demonstrate that Pb isotopes are efficient tools to trace the origin and the mobility of the contaminants in environments affected by uranium mining. PMID:27220101

  14. The importance of colloids and mires for the transport of uranium isotopes through the Kalix River watershed and Baltic Sea

    SciTech Connect

    Porcelli, D.; Wasserburg, G.J.; Andersson, P.S.

    1997-10-01

    The importance of colloids and organic deposits for the transport of uranium isotopes from continental source regions and through the estuarine environment was investigated in the mire-rich Kalix River drainage basin in northern Sweden and the Baltic Sea. Ultrafiltration techniques were used to separate uranium and other elements associated with colloids > 10 kD and >3 kD from {open_quotes}solute{close_quotes} uranium and provided consistent results and high recovery rates for uranium as well as for other elements from large volume samples. Uranium concentrations in 0.45 {mu}m-filtered Kalix River water samples increased by a factor of 3 from near the headwaters in the Caledonides to the river mouth while major cation concentrations were relatively constant. {sup 234}U {sup 238}U ratios were high ({delta}{sup 234}U = 770-1500) throughout the basin, without showing any simple pattern, and required a supply of {sup 234}U-rich water. Throughout the Kalix River, a large fraction (30-90%) of the uranium is carried by >10 kD colloids, which is compatible with uranium complexation with humic acids. No isotopic differences were found between colloid-associated and solute uranium. Within the Baltic Sea, about half of the uranium is removed at low salinities. The proportion that is lost is equivalent to that of river-derived colloid-bound uranium, suggesting that while solute uranium behaves conservatively during estuarine mixing, colloid-bound uranium is lost due to rapid flocculation of colloidal material. The association of uranium with colloids therefore may be an important parameter in determining uranium estuarine behavior. Mire peats in the Kalix River highly concentrate uranium and are potentially a significant source of recoil {sup 234}U to the mirewaters and river waters. However, mirewater data clearly demonstrate that only small {sup 234}U/{sup 238}U shifts are generated relative to inflowing groundwater. 63 refs., 8 figs., 3 tabs.

  15. Uranium-thorium isotope geochemistry of saline ground waters from central Missouri

    SciTech Connect

    Banner, J.L.; Chen, J.H.; Wasserburg, G.J.

    1989-03-01

    The isotopic and elemental distributions of uranium and thorium were examined in a suite of saline ground waters from central Missouri using mass spectrometric techniques. The waters were sampled from natural springs and artesian wells in Mississippian and Ordovician aquifers and have a wide range in salinity (5 to 26 /per thousand/), deltaD (/minus/108 to /minus/45 /per thousand/), and delta/sup 18/O (/minus/14.7 to /minus/6.5 /per thousand/) values. The suite of samples has a large range in /sup 238/U (50 to 200 x 10/sup /minus/12/g/g) and /sup 232/Th (0.3 to 9.1 x 10/sup /minus/12/g/g) concentrations and extremely high /sup 234/U//sup 238/U activity ratios ranging from 2.15 to 16.0. These isotopic compositions represent pronounced uranium-series disequilibrium compared with the value of modern seawater (1.15) or the equilibrium value (1.00). For such /sup 234/U-enriched waters, /sup 234/U//sup 238/U isotope ratios can be determined with a precision of /+-/ 10 /per thousand/ (2sigma) on 10 mL of sample and less than /+-/5 /per thousand/ on 100 mL. In contrast to the large /sup 234/U enrichments, /sup 230/Th//sup 238/U activity ratios in the ground waters are significantly lower than the equilibrium value. The more saline samples have markedly higher /sup 234/U//sup 238/U activity ratios and lower deltaD and delta/sup 18/O values. Unfiltered and filtered (< 0.1 ..mu..m) aliquots of a saline sample have the same isotopic composition and concentration of uranium, indicating uranium essentially occurs entirely as a dissolved species. The filtered/unfiltered concentration ratio for thorium in this sample is 0.29, demonstrating the predominant association of thorium with particulates.

  16. Uranium and lead isotopic stability in a metamict zircon under experimental hydrothermal conditions

    USGS Publications Warehouse

    Pidgeon, R.T.; O'Neil, J.R.; Silver, L.T.

    1966-01-01

    Disturbance of the uranium-lead isotopic system in a metamict Ceylon zircon has been produced in a 2 molal NaCl solution at 500??C and 1000 bars fluid pressure. Loss of radiogenic lead to the extent of 61 percent in 13 days was the most significant effect. The experimental results support the episodic rather than continuous lead-loss interpretation of natural zircon systems utilized in geochronology.

  17. Uranium isotope composition of a laterite profile during extreme weathering of basalt in Guangdong, South China

    NASA Astrophysics Data System (ADS)

    Huang, J.; Zhou, Z.; Gong, Y.; Lundstrom, C.; Huang, F.

    2015-12-01

    Rock weathering and soil formation in the critical zone are important for material cycle from the solid Earth to superficial system. Laterite is a major type of soil in South China forming at hot-humid climate, which has strong effect on the global uranium cycle. Uranium is closely related to the environmental redox condition because U is stable at U(Ⅳ) in anoxic condition and U(Ⅵ) as soluble uranyl ion (UO22+) under oxic circumstance. In order to understand the behavior of U isotopes during crust weathering, here we report uranium isotopic compositions of soil and base rock samples from a laterite profile originated from extreme weathering of basalt in Guangdong, South China. The uranium isotopic data were measured on a Nu Plasma MC-ICP-MS at the University of Illinois at Urbana-Champaign using the double spike method. The δ238U of BCR-1 is -0.29±0.03‰ (relative to the international standard CRM-112A), corresponding to a 238U/235U ratio of 137.911±0.004. Our result of BCR-1 agrees with previous analyses (e.g., -0.28‰ in Weyer et al. 2008) [1]. U contents of the laterite profile decrease from 1.9 ppm to 0.9 ppm with depth, and peak at 160 - 170 cm (2.3 ppm), much higher than the U content of base rocks (~0.5 ppm). In contrary, U/Th of laterites is lower than that of base rock (0.27) except the peak at the depth of 160-170 cm (0.38), indicating significant U loss during weathering. Notably, U isotope compositions of soils show a small variation from -0.38 to -0.28‰, consistent with the base rock within analytical error (0.05‰ to 0.08‰, 2sd). Such small variation can be explained by a "rind effect" (Wang et al., 2015) [2], by which U(Ⅳ) can be completely oxidized to U(VI) layer by layer during basalt weathering by dissolved oxygen. Therefore, our study indicates that U loss during basalt weathering at the hot-humid climate does not change U isotope composition of superficial water system. [1] Weyer S. et al. (2008) Natural fractionation of 238U/235

  18. Uranium Isotope Fractionation During Coprecipitation with Aragonite and Calcite

    NASA Astrophysics Data System (ADS)

    Chen, X.; Romaniello, S. J.; Herrmann, A. D.; Wasylenki, L. E.; Anbar, A. D.

    2014-12-01

    Natural variations in the 238U/235U ratio of marine carbonates may provide a useful way of constraining past variations in ocean redox conditions. However, before applying this novel redox proxy, it is essential to explore possible isotopic fractionation during U coprecipitation with aragonite and calcite. We investigated these effects in laboratory experiments. Aragonite and calcite coprecipitation experiments were conducted at pH 8.5±0.1 using a constant addition method [1]. More than 90% of the U was incorporated into the solid phase at the end of each experiment. Samples were purified using UTEVA chemistry and δ238/235U was measured using 233U-236U double-spike MC-ICP-MS with a precision of ±0.10‰ [2]. The aragonite experiment demonstrated a 238U/235U Rayleigh fractionation factor of α=1.00008±0.00002 with the 238U preferentially incorporated. In contrast, the calcite experiment demonstrated no resolvable U isotope fractionation (α=1.00001±0.00003). To determine if U isotopes are affected during the early diagenetic conversion of aragonite to calcite, natural carbonate samples were collected along an aragonite-calcite transition across a single coral head in the Key Largo limestone, and characterized for U concentration and δ238/235U [3]. We found that the mean δ238/235U in aragonite (-0.33±0.07‰ 2se) was slightly heavier than that in calcite (-0.37±0.02‰ 2se). Further work is needed to address the mechanisms leading to differential isotopic fractionation of U(VI) during incorporation into aragonite and calcite. Possible drivers include differences in coordination in the crystal structure or equilibrium isotopic fractionation between various aqueous U(VI) species prior to incorporation. [1] Reeder et al. (2001) GCA 65, 3491-3503. [2] Weyer et al., (2008) GCA 72, 345-359. [3] Gill et al., (2008) GCA 72, 4699-4722.

  19. Uranium isotopes in groundwater from the continental intercalaire aquifer in Algerian Tunisian Sahara (Northern Africa).

    PubMed

    Chkir, N; Guendouz, A; Zouari, K; Hadj Ammar, F; Moulla, A S

    2009-08-01

    The disequilibrium between (234)U and (238)U is commonly used as a tracer of groundwater flow. This paper aims to identify uranium contents and uranium isotopic disequilibria variation in groundwater sampled from deep Continental Intercalaire aquifer (southern Algeria and Tunisia). Large variations in both U contents (0.006-3.39ppb) and (234)U/(238)U activity ratios (0.4-15.38) are observed. We conduct a first assessment in order to verify whether the results of our investigation support and complete previous hydrogeological and isotopic studies. The dissolved U content and (234)U/(238)U activity ratio data were plotted on a two-dimensional diagram that was successfully utilized on sharing the CI aquifer into different compartments submitted to different oxidising/reducing conditions and leads also to distinguished two preferential flow paths in the Nefzaoua/Chott Fejej discharge area. Uranium isotopes disequilibrium indicate that ranium chemistry is mainly controlled by water-rock interaction enhanced by long residence time recognised for this aquifer. PMID:19559509

  20. Isotopic Tracking of Hanford 300 Area Derived Uranium in the Columbia River

    SciTech Connect

    Christensen, John N.; Dresel, P. Evan; Conrad, Mark E.; Patton, Gregory W.; DePaolo, Donald J.

    2010-10-31

    Our objectives in this study are to quantify the discharge rate of uranium (U) to the Columbia River from the Hanford Site's 300 Area, and to follow that U down river to constrain its fate. Uranium from the Hanford Site has variable isotopic composition due to nuclear industrial processes carried out at the site. This characteristic makes it possible to use high-precision isotopic measurements of U in environmental samples to identify even trace levels of contaminant U, determine its sources, and estimate discharge rates. Our data on river water samples indicate that as much as 3.2 kg/day can enter the Columbia River from the 300 Area, which is only a small fraction of the total load of dissolved natural background U carried by the Columbia River. This very low-level of Hanford derived U can be discerned, despite dilution to < 1 percent of natural background U, 350 km downstream from the Hanford Site. These results indicate that isotopic methods can allow the amounts of U from the 300 Area of the Hanford Site entering the Columbia River to be measured accurately to ascertain whether they are an environmental concern, or are insignificant relative to natural uranium background in the Columbia River.

  1. Absorption spectroscopy of uranium plasma for remote isotope analysis of next-generation nuclear fuel

    NASA Astrophysics Data System (ADS)

    Miyabe, M.; Oba, M.; Iimura, H.; Akaoka, K.; Maruyama, Y.; Ohba, H.; Tampo, M.; Wakaida, I.

    2013-07-01

    To determine experimental conditions suitable for isotope analysis, we studied the plume dynamics of uranium. A uranium oxide sample was ablated by 2nd harmonic radiation from a Nd:YAG laser at a fluence of 0.5 J/cm2. The temporal evolution of the ablation plume was investigated in vacuum and helium environments. In vacuum, the flow velocity perpendicular to the sample surface was determined to be 2.7 km/s for neutral atoms and 4.0 km/s for singly charged atoms. These velocities are about 20 % lower than those of cerium measured under similar conditions. From the evolution of the plume in helium, we found that an observation time of 3-5 μs and an observation height of about 2.5 mm are most suited for obtaining higher sensitivity. Observation times less than 3 μs were unsuitable for precise isotope analysis since the spectral modifications arising from the Doppler splitting effect are different between the two uranium isotopes. Using the established conditions, we evaluated the calibration curve linearity, limit of detection, and precision for three samples having different abundances of 235U.

  2. Isotopic Anomalies in a Uranium Cluster Formed by Lais

    NASA Astrophysics Data System (ADS)

    van de Walle, J.; Tarento, R. J.; Joyes, P.

    A study of a Au-U liquid alloy ion source (LAIS) where uranium is enriched in its lighter element (20% 235U, 80% 238U) has been performed by high resolution mass spectrometry. Monoatomic species Au+, Au2+, U2+, U3+ and polyatomic species Au+n, Up+n, AunU+ are observed. The monoatomic results are well explained by the Kingham postionization process. Au+n and AunU+ species present an interesting odd-even effect characteristic of monovalent elements. The main result of this preliminary letter is a heteroisotope anomaly which appears in U+2, U+3 and U4+3 emission where only homoisotopes are detected. A similar phenomenon was reported for Cu+2 and Ge+2 in a previous work and was attributed to a higher state of excitation of emitted heteroisotope aggregates which explode as they fly to the collector.1,2

  3. Improving the Sensitivity of Uranium Isotope Ratio Measurements

    NASA Astrophysics Data System (ADS)

    Friedrich, J.; Snow, J.

    2003-12-01

    Accurate and precise measurements of natural and anthropogenic 235/238 U isotope ratios are important for a range of investigations where the amount of sample is extremely restricted and/or the analyte is only present in ultra-trace quantities. Examples include biological, cosmochemical, environmental, geological, and radiological studies. We have developed and validated a novel method using our Nu Instruments Nu Plasma Multi Collector Inductively Coupled Plasma Mass Spectrometer (MC-ICPMS) and a 233U, 236U mixed double spike for the measurement of 235U/238U ratios. Our multi-dynamic technique employs the installed quadrupole zoom optics and fixed positioning of the ion counting detectors such that rather than the commonly used mass dispersion of 1 or 2, we utilize a mass dispersion of 1.5. Using this configuration, we can simultaneously monitor the 235U and 238U ion beams in the first cycle followed by a second cycle that simultaneously monitors the 233U and 236U beams. This innovative approach allows us to correct for the considerable, but consistent, instrumental mass fractionation and ion-counter amplification bias within each sequence. Since we were hesitant to use a U500 (235U, 238U equal atom) solution for spike calibration because of possible enriched U laboratory and instrumentation contamination, we used a U960 (terrestrial 235U/238U) solution for isotopic calibration of the spike. This standardization corrected for the small amounts of 235U and 238U in the spike solution by using a U960 standard solution. With a mean intraday 2-sigma precision of 1.5 permil and an overall 2-sigma precision of 2.25 permil using individual sample sizes of 350 pg (8.8 x10 E11 atoms), we are confident our technique will be useful for identifying U isotopic anomalies present in many sample types.

  4. CO-laser-induced photochemical reaction of UF6 with HCl for the isotope separation of uranium hexafluoride

    NASA Astrophysics Data System (ADS)

    Ding, Hong-Bin; Shen, Z. Y.; Zhang, Cun H.

    1993-05-01

    In this paper, we report the results of CO-laser induced photochemical reaction of UF6 with HCl for the isotope separation of uranium hexafluoride, we also discussed that the molecular collision inducing V-T, V-V relaxation process affects on the selectivity of the isotope separation. The obtained quantum coefficiency of the reaction is about 0.34.

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

    SciTech Connect

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

    2009-03-29

    Uranium (U) and plutonium (Pu) isotopes in coral soils, contaminated by nuclear weapons testing in the northern Marshall Islands, were isolated by ion-exchange chromatography and analyzed by mass spectrometry. The soil samples were spiked with {sup 233}U and {sup 242}Pu tracers, dissolved in minerals acids, and U and Pu isotopes isolated and purified on commercially available ion-exchange columns. The ion-exchange technique employed a TEVA{reg_sign} column coupled to a UTEVA{reg_sign} column. U and Pu isotope fractions were then further isolated using separate elution schemes, and the purified fractions containing U and Pu isotopes analyzed sequentially using multi-collector inductively coupled plasma mass spectrometer (MCICP-MS). High precision measurements of {sup 234}U/{sup 235}U, {sup 238}U/{sup 235}U, {sup 236}U/{sup 235}U, and {sup 240}Pu/{sup 239}Pu in soil samples were attained using the described methodology and instrumentation, and provide a basis for conducting more detailed assessments of the behavior and transfer of uranium and plutonium in the environment.

  6. U-Pb systems and U isotopic composition of the sandstone-hosted paleovalley Dybryn uranium deposit, Vitim uranium district, Russia

    NASA Astrophysics Data System (ADS)

    Golubev, V. N.; Chernyshev, I. V.; Chugaev, A. V.; Eremina, A. V.; Baranova, A. N.; Krupskaya, V. V.

    2013-11-01

    The isotopic (U-Pb, 238U-235U, 234U-238U) and chemical study of whole-rock samples and finegrained fractions of rocks in a vertical section of the terrigenous sequence at the Dybryn uranium deposit in the Khiagda ore field shows that a wide U-Pb isotopic age range (26.9-6.5 Ma) is caused by oxidation and disturbance of the U-Pb isotopic system in combination with protracted uranium ore deposition. The oxidation of rocks resulted in the loss of uranium relative to lead and eventually to an overestimated 206Pb/238U age at sites with a low U content. The 238U/235U ratios in the studied samples are within the range of 137.74-137.88. Samples with a high uranium content are characterized by a decreasing 238U/235U ratio with a decrease in 207Pb/235U and 206Pb/238U ages. A nonequilibrium 234U/238U ratio in most studied samples furnishes evidence for young (<1.5 Ma) transformation of the Miocene uranium ore, which is responsible for uranium migration and its redeposition.

  7. Fission track-secondary ion mass spectrometry as a tool for detecting the isotopic signature of individual uranium containing particles.

    PubMed

    Esaka, Fumitaka; Lee, Chi-Gyu; Magara, Masaaki; Kimura, Takaumi

    2012-04-01

    A fission track technique was used as a sample preparation method for subsequent isotope abundance ratio analysis of individual uranium containing particles with secondary ion mass spectrometry (SIMS) to measure the particles with higher enriched uranium efficiently. A polycarbonate film containing particles was irradiated with thermal neutrons and etched with 6M NaOH solution. Each uranium containing particle was then identified by observing fission tracks created and a portion of the film having a uranium containing particle was cut out and put onto a glassy carbon planchet. The polycarbonate film, which gave the increases of background signals on the uranium mass region in SIMS analysis, was removed by plasma ashing with 200 W for 20 min. In the analysis of swipe samples having particles containing natural (NBL CRM 950a) or low enriched uranium (NBL CRM U100) with the fission track-SIMS method, uranium isotope abundance ratios were successfully determined. This method was then applied to the analysis of a real inspection swipe sample taken at a nuclear facility. As a consequence, the range of (235)U/(238)U isotope abundance ratio between 0.0276 and 0.0438 was obtained, which was higher than that measured by SIMS without using a fission track technique (0.0225 and 0.0341). This indicates that the fission track-SIMS method is a powerful tool to identify the particle with higher enriched uranium in environmental samples efficiently. PMID:22405310

  8. Oxygen isotopic measurements by secondary ion mass spectrometry in uranium oxide microparticles: a nuclear forensic diagnostic.

    PubMed

    Tamborini, G; Phinney, D; Blidstein, O; Betti, M

    2002-12-01

    To exploit oxygen isotopic measurement by SIMS as a diagnostic tool in nuclear forensics, the magnitude and reproducibility of 0-isotope instrumental mass discrimination for O-isotope standards in the SIMS laboratory at the Institute for Transuranium Elements has been evaluated. Tests for matrix-dependent discrimination effects on three different O-isotope standards with substantially different matrix compositions have been performed. The results were checked by an interlaboratory comparison of O-isotope discrimination with those obtained in the SIMS laboratory at the Lawrence Livermore National Laboratory on two standards. The results from the two laboratories are in very good agreement, indicating statistically indistinguishable instrumental mass discrimination factors for 180/160 ratios on the Cameca 6f and 3f, when the analyses are performed under the experimental conditions described. The 2sigma(mean) uncertainties of these factors are in the range of 0.3-0.9%. In accordance with the tested methodology, 0-isotope compositions were measured in three particulate uranium oxide samples of nuclear forensics interest. PMID:12498207

  9. A Heterogeneous Sodium Fast Reactor Designed to Transmute Minor Actinide Actinide Waste Isotopes into Plutonium Fuel

    SciTech Connect

    Samuel E. Bays

    2011-02-01

    An axial heterogeneous sodium fast reactor design is developed for converting minor actinide waste isotopes into plutonium fuel. The reactor design incorporates zirconium hydride moderating rods in an axial blanket above the active core. The blanket design traps the active core’s axial leakage for the purpose of transmuting Am-241 into Pu-238. This Pu-238 is then co-recycled with the spent driver fuel to make new driver fuel. Because Pu-238 is significantly more fissile than Am-241 in a fast neutron spectrum, the fissile worth of the initial minor actinide material is upgraded by its preconditioning via transmutation in the axial targets. Because, the Am-241 neutron capture worth is significantly stronger in a moderated epithermal spectrum than the fast spectrum, the axial targets serve as a neutron trap which recovers the axial leakage lost by the active core. The sodium fast reactor proposed by this work is designed as an overall transuranic burner. Therefore, a low transuranic conversion ratio is achieved by a degree of core flattening which increases axial leakage. Unlike a traditional “pancake” design, neutron leakage is recovered by the axial target/blanket system. This heterogeneous core design is constrained to have sodium void and Doppler reactivity worth similar to that of an equivalent homogeneous design. Because minor actinides are irradiated only once in the axial target region; elemental partitioning is not required. This fact enables the use of metal targets with electrochemical reprocessing. Therefore, the irradiation environment of both drivers and targets was constrained to ensure applicability of the established experience database for metal alloy sodium fast reactor fuels.

  10. Groundwater salinization in the Saloum (Senegal) delta aquifer: minor elements and isotopic indicators.

    PubMed

    Faye, Serigne; Maloszewski, Piotr; Stichler, Willibald; Trimborn, Peter; Cissé Faye, Seynabou; Bécaye Gaye, Cheikh

    2005-05-01

    The hydrochemistry of minor elements bromide (Br), boron (B), strontium (Sr), environmental stable isotopes (18O and 2H) together with major-ion chemistry (chloride, sodium, calcium) has been used to constrain the source(s), relative age, and processes of salinization in the Continental Terminal (CT) aquifer in the Saloum (mid-west Senegal) region. Seventy-one groundwater wells which include 24 wells contaminated by saltwater and three sites along the hypersaline Saloum River were sampled to obtain additional information on the hydrochemical characteristics of the groundwater defined in previous studies. Use of Br against Cl confirms the Saloum River saline water intrusion up to a contribution of 7% into the aquifer. In addition to this recent intrusion, a relatively ancient intrusion of the Saloum River water which had reached at least as far as 20 km south from the source was evidenced. The high molar ratio values of Sr/Cl and Sr/Ca indicate an additional input of strontium presumably derived from carbonate precipitation/dissolution reactions and also via adsorption reactions. The variable B concentrations (7-650 microg/L) found in the groundwater samples were tested against the binary mixing model to evaluate the processes of salinization which are responsible for the investigated system. Sorption of B and depletion of Na occur as the Saloum river water intrudes the aquifer (salinization) in the northern part of the region, whereas B desorption and Na enrichment occur as the fresh groundwater flushing displaces the saline waters in the coastal strip (refreshening). In the central zone where ancient intrusion prevailed, the process of freshening of the saline groundwater is indicated by the changes in major-ion chemistry as well as B desorption and Na enrichment. In addition to these processes, stable isotopes reveal that mixing with recently infiltrating waters and evaporation contribute to the changes in isotopic signature. PMID:15862849

  11. Process for producing enriched uranium having a .sup.235 U content of at least 4 wt. % via combination of a gaseous diffusion process and an atomic vapor laser isotope separation process to eliminate uranium hexafluoride tails storage

    DOEpatents

    Horton, James A.; Hayden, Jr., Howard W.

    1995-01-01

    An uranium enrichment process capable of producing an enriched uranium, having a .sup.235 U content greater than about 4 wt. %, is disclosed which will consume less energy and produce metallic uranium tails having a lower .sup.235 U content than the tails normally produced in a gaseous diffusion separation process and, therefore, eliminate UF.sub.6 tails storage and sharply reduce fluorine use. The uranium enrichment process comprises feeding metallic uranium into an atomic vapor laser isotope separation process to produce an enriched metallic uranium isotopic mixture having a .sup.235 U content of at least about 2 wt. % and a metallic uranium residue containing from about 0.1 wt. % to about 0.2 wt. % .sup.235 U; fluorinating this enriched metallic uranium isotopic mixture to form UF.sub.6 ; processing the resultant isotopic mixture of UF.sub.6 in a gaseous diffusion process to produce a final enriched uranium product having a .sup.235 U content of at least 4 wt. %, and up to 93.5 wt. % or higher, of the total uranium content of the product, and a low .sup.235 U content UF.sub.6 having a .sup.235 U content of about 0.71 wt. % of the total uranium content of the low .sup.235 U content UF.sub.6 ; and converting this low .sup.235 U content UF.sub.6 to metallic uranium for recycle to the atomic vapor laser isotope separation process.

  12. Process for producing enriched uranium having a {sup 235}U content of at least 4 wt. % via combination of a gaseous diffusion process and an atomic vapor laser isotope separation process to eliminate uranium hexafluoride tails storage

    DOEpatents

    Horton, J.A.; Hayden, H.W. Jr.

    1995-05-30

    An uranium enrichment process capable of producing an enriched uranium, having a {sup 235}U content greater than about 4 wt. %, is disclosed which will consume less energy and produce metallic uranium tails having a lower {sup 235}U content than the tails normally produced in a gaseous diffusion separation process and, therefore, eliminate UF{sub 6} tails storage and sharply reduce fluorine use. The uranium enrichment process comprises feeding metallic uranium into an atomic vapor laser isotope separation process to produce an enriched metallic uranium isotopic mixture having a {sup 235} U content of at least about 2 wt. % and a metallic uranium residue containing from about 0.1 wt. % to about 0.2 wt. % {sup 235} U; fluorinating this enriched metallic uranium isotopic mixture to form UF{sub 6}; processing the resultant isotopic mixture of UF{sub 6} in a gaseous diffusion process to produce a final enriched uranium product having a {sup 235}U content of at least 4 wt. %, and up to 93.5 wt. % or higher, of the total uranium content of the product, and a low {sup 235}U content UF{sub 6} having a {sup 235}U content of about 0.71 wt. % of the total uranium content of the low {sup 235}U content UF{sub 6}; and converting this low {sup 235}U content UF{sub 6} to metallic uranium for recycle to the atomic vapor laser isotope separation process. 4 figs.

  13. Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

    SciTech Connect

    Maxwell, Sherrod L.; Hutchison, Jay B.; McAlister, Daniel R.

    2015-02-14

    Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, with total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.

  14. Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

    DOE PAGESBeta

    Maxwell, Sherrod L.; Hutchison, Jay B.; McAlister, Daniel R.

    2015-02-14

    Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, withmore » total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.« less

  15. Uranium, plutonium, and thorium isotopes in the atmosphere and the lithosphere

    SciTech Connect

    Essien, I.O.

    1983-01-01

    Concentration of /sup 238/U in rain and snow collected at Fayetteville (36/sup 0/N, 94/sup 0/W), Arkansas, showed a marked increase during the summer months of 1980, while Mount St. Helens remained active. This observed increase of /sup 238/U can be explained as due to the fallout of natural uranium from the eruption of Mount St. Helens. Large increases in the concentration of thorium isotopes detected in rain and snow samples during the last months of 1982 and early months of 1983 probably originated from the eruption of El Chichon volcano, which occurred on 28 March 1982. About 450 Ci of /sup 232/Th is estimated to have been injected into the atmosphere by this eruption. Isotopic anomalies were observed in atmospheric samples such as rain and snow. These anomalies can be attributed to various natural as well as man-made sources: nuclear weapon tests, nuclear accidents involving the burn-up of nuclear powered satellites, and volcanic eruptions. The variation of /sup 234/U//sup 238/U ratios in radioactive minerals when leached with nitric acid were also noticed and this variation, while /sup 235/U//sup 238/U remained fairly constant, can be explained in terms of the ..cap alpha..-recoil effect and changes in oxidation state of uranium. Difference found in /sup 239/Pu//sup 238/U ratios in terrestrial samples and uranium minerals can be explained as due to fallout contamination.

  16. Uranium series isotopes in the Avon Valley, Nova Scotia.

    PubMed

    Kronfeld, J; Godfrey-Smith, D I; Johannessen, D; Zentilli, M

    2004-01-01

    An U-series isotopic study was carried out in the waters of the Avon Valley, Nova Scotia. The fresh and acidic recharge waters flow rapidly through the watershed composed of a granitic highland and a sedimentary, largely carbonate, lowland plain, before draining to the sea. There is no significant anthropogenic pollution; but, naturally elevated U levels can be encountered within the bedrock. Nonetheless, the U concentrations of the surface and groundwater are low (generally within the range of several hundredths to several tenths of a microg l(-1)), except in the proximity to weathering of U mineralization. The dissolved U in the surface waters appears to be stabilized by organic rather than inorganic complexes. Both the groundwaters and surface waters have similar (234)U/(238)U activity ratios that rarely deviate from secular equilibrium by more than 20% throughout the watershed. The magnitude of the (234)U/(238)U activity ratio is not determined by lithology but rather by the weathering mechanism, the high rate of flushing, and the leaching of local U mineralization. Dissolved Ra is consistently absent. The dissolved Rn concentrations, though variable, are measurable even in surface waters. This may be due to a continual degassing from the U-enriched bedrock or release from local sites of U mineralization underlying the surface water sources. PMID:15050364

  17. Natural uranium and thorium isotopes in sediment cores off Malaysian ports

    NASA Astrophysics Data System (ADS)

    Yusoff, Abdul Hafidz; Sabuti, Asnor Azrin; Mohamed, Che Abd Rahim

    2015-06-01

    Sediment cores collected from three Malaysian marine ports, namely, Kota Kinabalu, Labuan and Klang were analyzed to determine the radioactivities of 234U, 238U, 230Th, 232Th and total organic carbon (TOC) content. The objectives of this study were to determine the factors that control the activity of uranium isotopes and identify the possible origin of uranium and thorium in these areas. The activities of 234U and 238U show high positive correlation with TOC at the middle of sediment core from Kota Kinabalu port. This result suggests that activity of uranium at Kota Kinabalu port was influenced by organic carbon. The 234U/238U value at the upper layer of Kota Kinabalu port was ≥1.14 while the ratio value at Labuan and Klang port was ≤ 1.14. These results suggest a reduction process occurred at Kota Kinabalu port where mobile U(VI) was converted to immobile U(IV) by organic carbon. Therefore, it can be concluded that the major input of uranium at Kota Kinabalu port is by sorptive uptake of authigenic uranium from the water column whereas the major inputs of uranium to Labuan and Klang port are of detrital origin. The ratio of 230Th/232Th was used to estimate the origin of thorium. Low ratio value (lt; 1.5) at Labuan and Klang ports support the suggestion that thorium from both areas were come from detrital input while the high ratio (> 1.5) of 230Th/232Th at Kota Kinabalu port suggest the anthropogenic input of 230Th to this area. The source of 230Th is probably from phosphate fertilizers used in the oil-palm cultivation in Kota Kinabalu that is adjacent to the Kota Kinabalu port.

  18. Design Study for a Low-Enriched Uranium Core for the High Flux Isotope Reactor, Annual report for FY 2009

    SciTech Connect

    Chandler, David; Freels, James D; Ilas, Germina; Miller, James Henry; Primm, Trent; Sease, John D; Guida, Tracey; Jolly, Brian C

    2010-02-01

    This report documents progress made during FY 2009 in studies of 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 alloy. With axial and radial grading 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 reactor performance from the current level. Results of selected benchmark studies imply that calculations of LEU performance are accurate. Studies are reported of the application of a silicon coating to surrogates for spheres of uranium-molybdenum alloy. A discussion of difficulties with preparing a fuel specification for the uranium-molybdenum alloy is provided. A description of the progress in developing a finite element thermal hydraulics model of the LEU core is provided.

  19. Determining the isotopic concentration of uranium from vector representation of the gamma spectrum

    NASA Astrophysics Data System (ADS)

    White, Tristan Glover

    Gamma emissions from Uranium-235 in a source of interest were compared to gamma emissions from Protactinium-234m (which is in equilibrium with Uranium-238) in order to determine the isotopic composition of the source. The 144 keV gamma ray from U-235 was compared with 1001 keV gamma ray from Pa-234m. Two analytical methods were compared: the relative activity method and the vector representation method. The relative activity method is similar to the (standard) relative intensity method, but accounts for more variables. Calculations were performed using both methods in order to evaluate precision and accuracy. Relative activity compares the number of counts under one gamma-ray peak from a reference source to the number of counts under another peak from an unknown source. This method is sensitive to systematic errors in the efficiency calibration of the detector when two different peaks with different energies are used. Vector representation compares the count ratio of two gamma-ray peaks from one source to the count ratio of the same two gamma-ray peaks from another source. Vector representation was found to be practical for analyzing depleted uranium, but not highly enriched uranium (HEU), due to different branching ratios and detector efficiency.

  20. Establishing Specifications for Low Enriched Uranium Fuel Operations Conducted Outside the High Flux Isotope Reactor Site

    SciTech Connect

    Pinkston, Daniel; Primm, Trent; Renfro, David G; Sease, John D

    2010-10-01

    The National Nuclear Security Administration (NNSA) has funded staff at Oak Ridge National Laboratory (ORNL) to study the conversion of the High Flux Isotope Reactor (HFIR) from the current, high enriched uranium fuel to low enriched uranium fuel. The LEU fuel form is a metal alloy that has never been used in HFIR or any HFIR-like reactor. This report provides documentation of a process for the creation of a fuel specification that will meet all applicable regulations and guidelines to which UT-Battelle, LLC (UTB) the operating contractor for ORNL - must adhere. This process will allow UTB to purchase LEU fuel for HFIR and be assured of the quality of the fuel being procured.

  1. Equilibrium uranium isotope fractionation by nuclear volume and mass-dependent processes

    NASA Astrophysics Data System (ADS)

    Schauble, E. A.

    2006-12-01

    Uranium serves as a geochemical tracer of oxidation near the Earth's surface, and is also the basis for several isotopic geochronometers. It is thus important to understand possible non-radiogenic and non-radioactive isotopic fractionation of uranium in natural systems. This study presents theoretical estimates of equilibrium uranium isotope fractionations in U-bearing molecules and complexes, calculated using first-principles computational chemistry. Ion-exchange experiments (1,2) have indicated that mass-dependent mechanisms, alone, cannot explain 238U/234U and 238U/^{235}U fractionations, so nuclear volume (i.e., field shift) fractionation effects are also considered in theoretical calculations. The results indicate that equilibrium isotopic fractionation is likely when U4+ and U6+ species equilibrate. Nuclear volume fractionation leads to higher 238U/^{235}U in U4+-bearing species, overwhelming a smaller mass- dependent fractionation in the opposite direction. The calculated net fractionation between U(H2O)_94+ and UO2Cl3(H2O)_2^- is approximately 1 per mil at 20-150°C, in agreement with earlier experiments. These results also reproduce the apparent non mass-dependent signature observed in 238U/234U relative to 238U/^{235}U. In addition to redox reactions, significant fractionation is expected between different U6+-bearing uranyl complexes (e.g., UO2(H2O)_52+, UO2(NO3)_3^-, UO2(CO3)(H2O)3). These results suggest that U-isotope composition could be used as a proxy for the oxidation state and speciation of natural waters, and that U-isotope ratios are not constant in materials formed or equilibrated at low temperatures. More generally, nuclear volume fractionations are expected to partially cancel or reverse mass-dependent fractionations caused by redox transitions among the high oxidation states (≥+2) of lanthanides, actinides, and heavy transition elements. References: 1. Nomura, Higuchi and Fujii, 1996, J. Am. Chem. Soc., v. 118, p. 9127-9130. 2. Bigeleisen

  2. Testing the Ortec's Isotopic and Eberlines Snap software for Uranium waste measurements

    SciTech Connect

    Vo, Duc T.; Seo, P. N.; Li, T. K.

    2003-01-01

    Uranium enrichment plants normally generate lots of wastes. The wastes are in various matrices such as clothing, glass, concrete, aluminum, and steel, etc. They are in the quantity of a few grams to many kilograms and generally stored in 55-gallon drums. For accountability, it is important to determine the amount of uranium in the waste drums to a certain level of accuracy. There are several commercially available systems that can accurately determine the uranium mass in the waste drums, such as Tomographic-Gamma-Scanner1 (TGS) or Segmented Gamma-Ray Scanner2 (SGS). However, those systems are too cumbersome and expensive. Cheap and simple single detector systems are also available commercially from several companies. The workhorse of these systems is the software, which would work with any germanium detector system. We mocked up waste drums containing several hundred grams to several kilograms of uranium with different isotopic compositions in various matrices. We acquired data using a coaxial germanium detector. We tested two different software codes from two companies, the Ortec's Isotopic software and the Eberline's Snap software. The results with the germanium detector were very encouraging, which led us to test with the NaI detectors. The NaI detectors have much worse resolution than the germanium detectors. However, they are very cheap, can be very large in detector size and, thus, efficient for a given counting time, and are simpler because of not requiring liquid nitrogen for cooling. The results, advantages, and disadvantages of the two software codes and the two detector systems will be discussed.

  3. Quantifying Uranium Isotope Ratios Using Resonance Ionization Mass Spectrometry: The Influence of Laser Parameters on Relative Ionization Probability

    SciTech Connect

    Isselhardt, Brett H.

    2011-09-01

    Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure relative uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process to provide a distinction between uranium atoms and potential isobars without the aid of chemical purification and separation. We explore the laser parameters critical to the ionization process and their effects on the measured isotope ratio. Specifically, the use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of 235U/238U ratios to decrease laser-induced isotopic fractionation. By broadening the bandwidth of the first laser in a 3-color, 3-photon ionization process from a bandwidth of 1.8 GHz to about 10 GHz, the variation in sequential relative isotope abundance measurements decreased from >10% to less than 0.5%. This procedure was demonstrated for the direct interrogation of uranium oxide targets with essentially no sample preparation. A rate equation model for predicting the relative ionization probability has been developed to study the effect of variation in laser parameters on the measured isotope ratio. This work demonstrates that RIMS can be used for the robust measurement of uranium isotope ratios.

  4. Development of a portable mass spectrometric system for determination of isotopic composition of solid uranium samples using fluorine volatilization

    NASA Astrophysics Data System (ADS)

    Loge, G.

    1994-09-01

    Using hardware and materials supplied by LANL, a prototype quadrupole mass spectrometer system designed for portable field analysis of isotopic composition of solid uranium samples was assembled and tested. The system contained the capability for fluorine volatilization of solid uranium samples with gas introduction, which was successfully tested and demonstrated using 100 mg samples of U3O8. Determination of precision and accuracy for measuring isotopic composition was performed using isotopic standards. Use with soil samples containing uranium were also attempted. Silicates in the soil forming SiF4 were found to be a kinetic bottleneck to the formation of UF6. This could be avoided by performing some sort of chemical separation as a pre-treatment step, which was demonstrated using nitric acid.

  5. Isotopic analysis of uranium in U3O8 by passive gamma-ray spectrometry

    PubMed

    Nir-El

    2000-03-01

    Passive gamma-ray spectrometry was applied to analyze the isotopic composition of uranium in U3O8. Depleted and enriched U3O8 standard reference materials were used to calibrate the system. An independent calibration was performed by standard gamma-ray point sources. U3O8 SRM samples of the 950 series were analyzed. The present results show that the isotopic abundances of 235U in SRMs 950, 950a and 950b are higher by +3.6, +0.9 and +0.9% (relative deviation) than the natural value 0.7200%, while relative precisions were +/-0.4, +/-0.7 and +/-0.3%, respectively. PMID:10724436

  6. High Precision Measurements of 235U/238U Isotopic Fractionations Resulting From Uranium Reduction Induced by Zero Valent Iron

    NASA Astrophysics Data System (ADS)

    Rademacher, L.; Lundstrom, C.; Johnson, T.

    2003-12-01

    Uranium is a widespread natural and anthropogenic contaminant in surface and subsurface waters. Like several other inorganic contaminants, uranium is mobile under oxidizing conditions but may be immobilized by chemical reduction. U(VI) moves with groundwater as (UO2)2+ and as soluble complexes with carbonate, phosphate, and fluoride. In many groundwater systems, uranium undergoes chemical reduction to U(IV), which is insoluble and immobile. Therefore, understanding the extent of reduction is essential for predicting the mobility of uranium in groundwater. Mass dependent isotopic fractionations of redox sensitive contaminants frequently found in groundwater (including chromate, selenate, and nitrate) have proven exceptionally useful for estimating the rate and extent of reduction and immobilization. Until recently, however, analytical limitations have prevented these techniques from being applied to heavier redox sensitive elements, such as uranium. The advent of highly sensitive multi-collector inductively coupled plasma mass spectrometers (MC-ICP-MS) enables high precision measurements of previously undetected variations in many elements. Laboratory reduction experiments with zero valent iron (ZVI) were performed in a controlled environment to test the hypothesis that uranium isotopes, specifically 235U/238U, behave similarly to other redox sensitive contaminants and produce a mass dependent fractionation during the transformation between valence states. Because of the large abundance differences between 235U and 238U, initial experiments used U500, an enriched uranium standard with approximately equal parts 235U and 238U. Results suggest that the highly sensitive MC-ICP-MS distinguishes 235U/238Uvariations to approximately + 0.02per mil. Measured isotopic fractionations between the 235U/238U of the initial and final experimental solutions (~70% reduced) are approximately 1.1 per mil, and increase with decreasing concentration. Measured variations in 235U/238U

  7. Isotopic determination of uranium in soil by laser induced breakdown spectroscopy

    NASA Astrophysics Data System (ADS)

    Chan, George C.-Y.; Choi, Inhee; Mao, Xianglei; Zorba, Vassilia; Lam, Oanh P.; Shuh, David K.; Russo, Richard E.

    2016-08-01

    Laser-induced breakdown spectroscopy (LIBS) operated under ambient pressure has been evaluated for isotopic analysis of uranium in real-world samples such as soil, with U concentrations in the single digit percentage levels. The study addresses the requirements for spectral decomposition of 235U and 238U atomic emission peaks that are only partially resolved. Although non-linear least-square fitting algorithms are typically able to locate the optimal combination of fitting parameters that best describes the experimental spectrum even when all fitting parameters are treated as free independent variables, the analytical results of such an unconstrained free-parameter approach are ambiguous. In this work, five spectral decomposition algorithms were examined, with different known physical properties (e.g., isotopic splitting, hyperfine structure) of the spectral lines sequentially incorporated into the candidate algorithms as constraints. It was found that incorporation of such spectral-line constraints into the decomposition algorithm is essential for the best isotopic analysis. The isotopic abundance of 235U was determined from a simple two-component Lorentzian fit on the U II 424.437 nm spectral profile. For six replicate measurements, each with only fifteen laser shots, on a soil sample with U concentration at 1.1% w/w, the determined 235U isotopic abundance was (64.6 ± 4.8)%, and agreed well with the certified value of 64.4%. Another studied U line - U I 682.691 nm possesses hyperfine structure that is comparatively broad and at a significant fraction as the isotopic shift. Thus, 235U isotopic analysis with this U I line was performed with spectral decomposition involving individual hyperfine components. For the soil sample with 1.1% w/w U, the determined 235U isotopic abundance was (60.9 ± 2.0)%, which exhibited a relative bias about 6% from the certified value. The bias was attributed to the spectral resolution of our measurement system - the measured line

  8. Time Constraints on Soil Evolution from Uranium-series Isotopes in the South-eastern Australian Highlands: Evidences for a Coupling Between Soil Erosion and Production

    NASA Astrophysics Data System (ADS)

    Puthiyaveetil Othayoth, S.; Dosseto, A.; Hesse, P. P.; Handley, H. K.

    2011-12-01

    The evolution of soil resources (steady-state, aggradation or degradation) is determined by the balance between soil production and denudation rates. The uranium-series isotopic composition of four soil profiles from Frogs Hollow, a location in the upper catchment area of the Murrumbidgee River in southeastern Australia, has been determined to constrain the soil production rate in this region. The results are compared with previous estimates of soil residence time at this site, estimated from cosmogenic radionuclides and soil elemental chemistry data. Soil is increasingly weathered from bottom to top, which is evident from the decrease in (234U/238U) ratios and increase in relative quartz content with decreasing soil depth. The observed variations in mineralogy and geochemistry between the four soil profiles reflect differences in the degree of weathering. Sequential leaching was conducted to assess how uranium-series isotopes are distributed between primary and secondary minerals. Leached and unleached aliquots show similar mineralogy with minor variation in the relative mineral abundances whereas the elemental and isotopic compositions of uranium and thorium show notable differences. The unleached samples show more systematic variations in uranium-series isotopic compositions with depth when compared to leached samples. Soil residence times are calculated by modeling soil uranium-series isotopic composition using the model from (Dosseto et al., 2008). Inferred values vary from 3 to 30 kyr for profiles F1 (unleached aliquots) and F2. A negative correlation is observed between muscovite abundance and calculated soil residence times. The slope of this correlation is similar for different soil profiles and for both leached and unleached aliquots. Thus, we were able to apply this relationship to profiles where the residence time could not be calculated due to scatter in U-series isotope compositions. The inferred soil residence times range from 3 to 33 kyr for leached

  9. Mechanisms of magma generation beneath hawaii and mid-ocean ridges: uranium/thorium and samarium/neodymium isotopic evidence.

    PubMed

    Sims, K W; Depaolo, D J; Murrell, M T; Baldridge, W S; Goldstein, S J; Clague, D A

    1995-01-27

    Measurements of uranium/thorium and samarium/neodymium isotopes and concentrations in a suite of Hawaiian basalts show that uranium/thorium fractionation varies systematically with samarium/neodymium fractionation and major-element composition; these correlations can be understood in terms of simple batch melting models with a garnet-bearing peridotite magma source and melt fractions of 0.25 to 6.5 percent. Midocean ridge basalts shows a systematic but much different relation between uranium/thorium fractionation and samarium/neodymium fractionation, which, although broadly consistent with melting of a garnet-bearing peridotite source, requires a more complex melting model. PMID:17788786

  10. DESIGN STUDY FOR A LOW-ENRICHED URANIUM CORE FOR THE HIGH FLUX ISOTOPE REACTOR, ANNUAL REPORT FOR FY 2010

    SciTech Connect

    Cook, David Howard; Freels, James D; Ilas, Germina; Jolly, Brian C; Miller, James Henry; Primm, Trent; Renfro, David G; Sease, John D; Pinkston, Daniel

    2011-02-01

    This report documents progress made during FY 2010 in studies of 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 alloy. With axial and radial grading 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 level. Studies are reported of support to a thermal hydraulic test loop design, the implementation of finite element, thermal hydraulic analysis capability, and infrastructure tasks at HFIR to upgrade the facility for operation at 100 MW. A discussion of difficulties with preparing a fuel specification for the uranium-molybdenum alloy is provided. Continuing development in the definition of the fuel fabrication process is described.

  11. Partial Safety Analysis for a Reduced Uranium Enrichment Core for the High Flux Isotope Reactor

    SciTech Connect

    Primm, Trent; Gehin, Jess C

    2009-04-01

    A computational model of the reactor core of the High Flux Isotope Rector (HFIR) was developed in order to analyze non-destructive accidents caused by transients during reactor operation. The reactor model was built for the latest version of the nuclear analysis software package called Program for the Analysis of Reactor Transients (PARET). Analyses performed with the model constructed were compared with previous data obtained with other tools in order to benchmark the code. Finally, the model was used to analyze the behavior of the reactor under transients using a different nuclear fuel with lower enrichment of uranium (LEU) than the fuel currently used, which has a high enrichment of uranium (HEU). The study shows that the presence of fertile isotopes in LEU fuel, which increases the neutron resonance absorption, reduces the impact of transients on the fuel and enhances the negative reactivity feedback, thus, within the limitations of this study, making LEU fuel appear to be a safe alternative fuel for the reactor core.

  12. Reaction paths and host phases of uranium isotopes (235U; 238U), Saanich Inlet

    NASA Astrophysics Data System (ADS)

    Amini, M.; Holmden, C. E.; Francois, R. H.

    2009-12-01

    In recent times, Uranium has become increasingly the focus of stable isotope fractionation studies. Variations in 238U/235U have been reported as a result of redox reactions [1,2] from the nuclear field shift effect [3], and a mass-dependent, microbially-mediated, kinetic isotope effect [4]. The 238U/235U variability caused by changes in environmental redox conditions leads to an increase in the 238U/235U ratios of the reduced U species sequestered into marine sediments. This points to U isotope variability as a new tool to study ancient ocean redox changes. However, the process by which reduced sediments become enriched in the heavy isotopes of U is not yet known, and hence the utility of 238U/235U as a redox tracer remains to be demonstrated. In order to further constrain sedimentary U enrichment and related isotope effect, we are investigating U isotopic compositions of water samples and fresh surface sediment grab samples over a range of redox conditions in the seasonally anoxic Saanich Inlet, on the east coast of Vancouver Island. U was sequentially extracted from sediments in order to characterize specific fractions for their isotopic composition. The measurements were carried out by MC-ICPMS using 233U/236U-double spike technique. The data are reported as δ238U relative to NBL 112a with a 238U/235U ratio of 137.88 (2sd). External precision is better than 0.10‰ (2sd). Fifteeen analyses of seawater yielded δ238U of -0.42±0.08‰ (2sd). The results for the water samples indicate a homogenous δ238U value throughout the Saanich Inlet water column that matches the global seawater signature. All of the water samples from above and below average -0.42±0.05‰ (2sd). In contrast, a plankton net sample yielded a distinctly different, (about 0.5‰ lighter) isotope value. Bacterial reduction experiments [4] have also shown isotope enrichment factors of about -0.3‰. In addition, metal isotope fractionation occurs during adsorption with the light isotope being

  13. Sulfur Isotopes as Indicators of Bacterial Sulfate Reduction Processes Influencing Field Scale Uranium Bioremediation

    NASA Astrophysics Data System (ADS)

    Druhan, J. L.; Conrad, M. E.; Williams, K. H.; N'guessan, L.; Long, P. E.; Hubbard, S. S.

    2007-12-01

    An in-situ acetate amendment at a DOE Uranium Mill Tailings Remedial Action (UMTRA) site near Rifle, CO demonstrated successful reduction of aqueous U(VI), to less soluble U(IV) through stimulated microbial activity. U(VI) reduction rates were highest during iron reduction and decreased with the onset of sulfate reduction. However, sustained U(IV) attenuation was observed following subsequent termination of the acetate amendment. These findings illustrate the importance of the transition between iron and sulfate reducing conditions in stimulating bioreduction of uranium. The sulfur isotope compositions of sulfate and sulfide were measured through this transition in order to explore the utility of these data in tracking the extent of microbial sulfate reduction and to assess the stability of sulfide precipitates. Samples for isotopic analyses and aqueous measurements of sulfate, ferrous iron, U(VI) and acetate were collected in one background well and three monitoring wells down-gradient of the acetate injection. Results show an increase of up to 7‰ in the δ34S of sulfate at the onset of sulfate reduction, followed by a return to background δ34S values of -8‰ following cessation of the acetate amendment. The δ34S values of sulfide increased from roughly -20‰ at the onset of sulfate reduction to a maximum of -0.8‰ during peak sulfate removal, followed by a gradual return to values of roughly -28‰ upon cessation of the acetate amendment. These data present a unique perspective on the processes governing the bioreduction experiment in that the sulfate isotopes are a function of both transport and mixing processes, whereas the sulfide isotopes represent biogenic sulfide that is rapidly removed from the aqueous phase. Thus a comparable enrichment in sulfate isotopic data noted in the closest and furthest wells from the injection gallery suggest bioreduction in both of these locations, while a larger increase in sulfide isotopic values in the closest well

  14. Uranium and thorium isotopes and their state of equilibria in lungs from uranium miners.

    PubMed

    Wrenn, M E; Singh, N P; Saccomanno, G

    1983-01-01

    Radiochemical analysis of seven lungs obtained at autopsy show that concentrations ranged between 6 and 63 pCi/kg for 238U and 6-66 pCi/kg, for 234U. Similarly, 230Th ranged from 17 to 54 pCi/kg, two orders of magnitude higher than 230Th observed in the lungs of the general population from the Western mining region. For individual lungs, 238U and 234U were close to equilibrium with an average ratio of 238U/234U of 0.94 and a range of 0.80-1.02. Surprisingly, 230Th was close to equilibrium with 234U with a 230Th/234U ratio of 1.1 and a range from 0.54 to 2.6. Equilibrium between U and Th isotopes is in contrast to the disequilibrium reported in beagles which chronically inhaled carnotite, where the 230Th/234U ratio was observed to range from 5.4 to 7.4 with an average of 6.3. The average radiation dose rate to lung from each of the three radionuclides was calculated as follows: D = 18.7 CE where D = dose rate in mrad/year, C = activity concentration in tissue in pCi/g and E = energy absorbed per disintegration in MeV. The combined radiation dose rate (at death) due to three long-lived radionuclides 238U, 234U and 230Th varied from 2.5 to 14.2 mrad/yr with a mean of 9.6 mrad/yr. The concentration of 226Ra and daughters in the lung was not determined. An upper limit to the dose rate from the whole chain, calculated assuming 226Ra through 210Po are in equilibrium with 238U, 234U and 230Th, would be 30 mrad/yr. PMID:6862915

  15. Heterogeneous sodium fast reactor designed for transmuting minor actinide waste isotopes into plutonium fuel

    NASA Astrophysics Data System (ADS)

    Bays, Samuel Eugene

    2008-10-01

    In the past several years there has been a renewed interest in sodium fast reactor (SFR) technology for the purpose of destroying transuranic waste (TRU) produced by light water reactors (LWR). The utility of SFRs as waste burners is due to the fact that higher neutron energies allow all of the actinides, including the minor actinides (MA), to contribute to fission. It is well understood that many of the design issues of LWR spent nuclear fuel (SNF) disposal in a geologic repository are linked to MAs. Because the probability of fission for essentially all the "non-fissile" MAs is nearly zero at low neutron energies, these isotopes act as a neutron capture sink in most thermal reactor systems. Furthermore, because most of the isotopes produced by these capture reactions are also non-fissile, they too are neutron sinks in most thermal reactor systems. Conversely, with high neutron energies, the MAs can produce neutrons by fast fission. Additionally, capture reactions transmute the MAs into mostly plutonium isotopes, which can fission more readily at any energy. The transmutation of non-fissile into fissile atoms is the premise of the plutonium breeder reactor. In a breeder reactor, not only does the non-fissile "fertile" U-238 atom contribute fast fission neutrons, but also transmutes into fissile Pu-239. The fissile value of the plutonium produced by MA transmutation can only be realized in fast neutron spectra. This is due to the fact that the predominate isotope produced by MA transmutation, Pu-238, is itself not fissile. However, the Pu-238 fission cross section is significantly larger than the original transmutation parent, predominately: Np-237 and Am-241, in the fast energy range. Also, Pu-238's fission cross section and fission-to-capture ratio is almost as high as that of fissile Pu-239 in the fast neutron spectrum. It is also important to note that a neutron absorption in Pu-238, that does not cause fission, will instead produce fissile Pu-239. Given this

  16. Weathering and transport of sediments in the Bolivian Andes: Time constraints from uranium-series isotopes

    NASA Astrophysics Data System (ADS)

    Dosseto, A.; Bourdon, B.; Gaillardet, J.; Maurice-Bourgoin, L.; Allègre, C. J.

    2006-08-01

    Rivers from the upper Rio Madeira basin (Bolivia) have been studied with uranium-series isotopes in order to constrain the timescales of weathering and sediment transfer from the Andes through the Amazon tropical plain. Uranium (U), thorium (Th) and radium (Ra) isotopes ( 238U- 234U- 230Th- 226Ra and 232Th) have been analyzed in the suspended load (> 0.2 μm) of rivers. Increasing 230Th excesses relative to 238U in suspended particles from the Andes to the tropical plain is interpreted as an increasing duration of weathering during sediment transport and storage in the foreland basin. Model calculations for ( 230Th/ 238U) and ( 226Ra/ 230Th) activity ratios in suspended particles using a continuous weathering model indicates that: (i) the timescale for production, storage and transport of sediments in the Andean Cordillera is only a few kyr, (ii) the storage time of suspended sediments in the foreland basin is 5 ± 1 kyr and (iii) the average transfer time of suspended sediments from the Andes to the confluence of Rio Madeira with the Amazon River is 17 ± 3 kyr. An implication of these short timescales is that the bedrock eroded must have lost part of its uranium during one or several past erosion cycles. This demonstrates the recycling of sediments through several erosion cycles before transfer to the oceans. The calculation of long-term (> 1 kyr), steady-state erosion rates indicates that they are much lower than present-day rates. This increase in denudation rates must be recent and could be explained by an increase in precipitation ˜ 4 ka ago, as suggested by palaeoclimatic evidences and the draining of transient sedimentary basins encountered on the Altiplano and easily eroded. This suggests that climatic variability rather than tectonics alone produces high erosion rates.

  17. Uranium Bio-accumulation and Cycling as revealed by Uranium Isotopes in Naturally Reduced Sediments from the Upper Colorado River Basin

    NASA Astrophysics Data System (ADS)

    Lefebvre, Pierre; Noël, Vincent; Jemison, Noah; Weaver, Karrie; Bargar, John; Maher, Kate

    2016-04-01

    Uranium (U) groundwater contamination following oxidized U(VI) releases from weathering of mine tailings is a major concern at numerous sites across the Upper Colorado River Basin (CRB), USA. Uranium(IV)-bearing solids accumulated within naturally reduced zones (NRZs) characterized by elevated organic carbon and iron sulfide compounds. Subsequent re-oxidation of U(IV)solid to U(VI)aqueous then controls the release to groundwater and surface water, resulting in plume persistence and raising public health concerns. Thus, understanding the extent of uranium oxidation and reduction within NRZs is critical for assessing the persistence of the groundwater contamination. In this study, we measured solid-phase uranium isotope fractionation (δ238/235U) of sedimentary core samples from four study sites (Shiprock, NM, Grand Junction, Rifle and Naturita, CO) using a multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS). We observe a strong correlation between U accumulation and the extent of isotopic fractionation, with Δ238U up to +1.8 ‰ between uranium-enriched and low concentration zones. The enrichment in the heavy isotopes within the NRZs appears to be especially important in the vadose zone, which is subject to variations in water table depth. According to previous studies, this isotopic signature is consistent with biotic reduction processes associated with metal-reducing bacteria. Positive correlations between the amount of iron sulfides and the accumulation of reduced uranium underline the importance of sulfate-reducing conditions for U(IV) retention. Furthermore, the positive fractionation associated with U reduction observed across all sites despite some variations in magnitude due to site characteristics, shows a regional trend across the Colorado River Basin. The maximum extent of 238U enrichment observed in the NRZ proximal to the water table further suggests that the redox cycling of uranium, with net release of U(VI) to the groundwater by

  18. Uranium isotope fractionation in Saanich Inlet: A modern analog study of a paleoredox tracer

    NASA Astrophysics Data System (ADS)

    Holmden, C.; Amini, M.; Francois, R.

    2015-03-01

    Uranium isotope fractionation was studied in the sediment and water of Saanich Inlet, a seasonally anoxic fjord on the east coast of Vancouver Island. The concentration of dissolved U is the same above and below the redoxcline at ˜120 m depth, with an average δ238U value of -0.45 ± 0.06‰ (2 s.e.), which is indistinguishable from seawater values reported in other studies. This finding is consistent with water renewal times for the inlet that are roughly seasonal in frequency, thus hiding the impact of the U losses to the anoxic sediment of the inlet. Complete digests of the anoxic sediment yielded higher δ238U values than seawater (-0.21 ± 0.11‰ (2 s.e.)). By contrast, complete digests of the sediment trap samples yielded lower δ238U values than seawater (-0.52 ± 0.10‰ (2 s.e.)), and marine plankton from the inlet yielded the lowest δ238U value of -1.24 ± 0.17‰ (2σ). Cross-plots of δ238U and δ234U vs. Th/U reveal strong correlations indicative of two-component mixing when the data from traps and anoxic inlet sediment are combined. One mixing end-member is fractionated uranium of seawater origin, with a δ238U value of 0.17 ± 0.14‰ (2σ). The other is detrital uranium with a δ238U value of -0.83 ± 0.12‰ (2σ). The detrital end-member is lower than the range of δ238U values reported in the literature for granitoid igneous rocks (-0.44‰ to -0.17‰, 2σ) (Telus et al., 2012), suggesting that continental weathering fractionates uranium isotopes, with preferential release of 238U. Development and application of U isotopes as a paleoredox proxy has its basis in the nuclear volume fractionation. The data from Saanich Inlet meets this expectation, with a positive fractionation factor (Δaq(VI)sed(IV)) of 0.62 ± 0.17‰ (2σ) calculated as the difference in δ238U between authigenic U in anoxic sediments and sediment traps (+0.17‰) and U dissolved in seawater (-0.45‰). However, it is widely believed that U(VI) reduction in the marine

  19. Uranium isotopes distinguish two geochemically distinct stages during the later Cambrian SPICE event

    NASA Astrophysics Data System (ADS)

    Dahl, Tais W.; Boyle, Richard A.; Canfield, Donald E.; Connelly, James N.; Gill, Benjamin C.; Lenton, Timothy M.; Bizzarro, Martin

    2014-09-01

    Anoxic marine zones were common in early Paleozoic oceans (542-400 Ma), and present a potential link to atmospheric pO2 via feedbacks linking global marine phosphorous recycling, primary production and organic carbon burial. Uranium (U) isotopes in carbonate rocks track the extent of ocean anoxia, whereas carbon (C) and sulfur (S) isotopes track the burial of organic carbon and pyrite sulfur (primary long-term sources of atmospheric oxygen). In combination, these proxies therefore reveal the comparative dynamics of ocean anoxia and oxygen liberation to the atmosphere over million-year time scales. Here we report high-precision uranium isotopic data in marine carbonates deposited during the Late Cambrian ‘SPICE’ event, at ca. 499 Ma, documenting a well-defined -0.18‰ negative δ238U excursion that occurs at the onset of the SPICE event's positive δ13C and δ34S excursions, but peaks (and tails off) before them. Dynamic modelling shows that the different response of the U reservoir cannot be attributed solely to differences in residence times or reservoir sizes - suggesting that two chemically distinct ocean states occurred within the SPICE event. The first ocean stage involved a global expansion of euxinic waters, triggering the spike in U burial, and peaking in conjunction with a well-known trilobite extinction event. During the second stage widespread euxinia waned, causing U removal to tail off, but enhanced organic carbon and pyrite burial continued, coinciding with evidence for severe sulfate depletion in the oceans (Gill et al., 2011). We discuss scenarios for how an interval of elevated pyrite and organic carbon burial could have been sustained without widespread euxinia in the water column (both non-sulfidic anoxia and/or a more oxygenated ocean state are possibilities). Either way, the SPICE event encompasses two different stages of elevated organic carbon and pyrite burial maintained by high nutrient fluxes to the ocean, and potentially sustained by

  20. Uranium and minor-element partitioning in Fe-Ti oxides and zircon from partially melted granodiorite, Crater Lake, Oregon

    SciTech Connect

    La Tourrette, T.Z.; Burnett, D.S. ); Bacon C.R. )

    1991-02-01

    Crystal-liquid partitioning in Fe-Ti oxides and zircon was studied in partially melted granodiorite blocks ejected during the climactic eruption of Mt. Mazama (Crater Lake), Oregon. The blocks, which contain up to 33% rhyolite glass (75 wt% SiO{sub 2}), are interpreted to be portions of the magma chamber walls that were torn off during eruption. The glass is clear and well homogenized for all measured elements except Zr. Results for Fe-Ti oxides give D{sub U}{sup oxide/liq} {approx} 0.1. Partitioning of Mg, Mn, Al, Si, V, and Cr in Fe-Ti oxides indicates that grains surrounded by glass are modestly well equilibrated with the melt for many of the minor elements, while those that are inclusions in relict plagioclase are not. Uranium and ytterbium inhomogeneities in zircons indicate that the zircons have only partially equilibrated with the melt and that uranium appears to have been diffusing out of the zircons have only partially equilibrated with the melt and that uranium appears to have been diffusing out of the zircons faster that the zircons were dissolving. Based on the authors measurements and given their low abundances in most rocks, Fe-Ti oxides probably do not play a major role in U-Th fractional during partial melting. The partial melts were undersaturated with zircon and apatite, but both phases are present in the authors samples. This demonstrates an actual case of nonequilibrium source retention of accessory phases, which in general could be an important trace element fractionation mechanism. Their results do not support the hypothesis that liquid structure is the dominant factor controlling trace-element partitioning in high-silica rhyolites.

  1. The isotopic composition of uranium and lead in Allende inclusions and meteoritic phosphates

    NASA Technical Reports Server (NTRS)

    Chen, J. H.; Wasserburg, G. J.

    1981-01-01

    The isotopic compositions of uranium and lead in Ca-Al-rich inclusions from the Allende chondrite and in whitlockite from the St. Severin chondrite and the Angra dos Reis achondrite are reported. Isoptopic analysis of acid soluble fractions of the Allende inclusions and the meteoritic whitlockite, which show isotopic anomalies in other elements, reveals U-235/U-238 ratios from 1/137.6 to 1/138.3, within 20 per mil of normal terrestrial U abundances. The Pb isotopic compositions of five coarse-grained Allende inclusions give a mean Pb-207/Pb-206 model age of 4.559 + or - 0.015 AE, in agreement with the U results. Pb isotope ratios of two fine-grained inclusions and a coarse-grained inclusion with strong mass fractionation and some nonlinear isotopic anomalies indicate that the U-Pb systems of these inclusions have evolved differently from the rest of Allende. Th/U abundance ratios in the Allende inclusions and meteoritic phosphate are found to range from 3.8 to 96, presumably indicating an optimal case for Cm/U fractionation, although the normal U concentrations do not support claims of abundant live Cm-247 or Cm-247/U-238 fractionation at the time of meteorite formation, in contrast to previous results. A limiting Cm-247/U-235 ratio of 0.004 at the time of meteorite formation is calculated which implies that the last major r process contribution at the protosolar nebula was approximately 100 million years prior to Al-26 formation and injection.

  2. Concentrations and activity ratios of uranium isotopes in groundwater from Donana National Park, South of Spain

    SciTech Connect

    Bolivar, J. P.; Olias, M.; Gonzalez-Garcia, F.; Garcia-Tenorio, R.

    2008-08-07

    The levels and distribution of natural radionuclides in groundwaters from the unconfined Almonte-Marismas aquifer, upon which Donana 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 {sup 210}Po), 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 {sup 234}U/{sup 238}U 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.

  3. Third Minima in Thorium and Uranium Isotopes in a Self-Consistent Theory

    SciTech Connect

    McDonnell, J. D.

    2013-01-01

    Background: Well-developed third minima, corresponding to strongly elongated and reflection-asymmetric shapes associated with dimolecular configurations, have been predicted in some non-self-consistent models to impact fission pathways of thorium and uranium isotopes. These predictions have guided the interpretation of resonances seen experimentally. On the other hand, self-consistent calculations consistently predict very shallow potential-energy surfaces in the third minimum region.

    Purpose: We investigate the interpretation of third-minimum configurations in terms of dimolecular (cluster) states. We study the isentropic potential-energy surfaces of selected even-even thorium and uranium isotopes at several excitation energies. In order to understand the driving effects behind the presence of third minima, we study the interplay between pairing and shell effects.

    Methods: We use the finite-temperature superfluid nuclear density functional theory. We consider two Skyrme energy density functionals: a traditional functional SkM and a recent functional UNEDF1 optimized for fission studies.

    Results: We predict very shallow or no third minima in the potential-energy surfaces of 232Th and 232U. In the lighter Th and U isotopes with N = 136 and 138, the third minima are better developed. We show that the reflection-asymmetric configurations around the third minimum can be associated with dimolecular states involving the spherical doubly magic 132Sn and a lighter deformed Zr or Mo fragment. The potential-energy surfaces for 228,232Th and 232U at several excitation energies are presented. We also study isotopic chains to demonstrate the evolution of the depth of the third minimum with neutron number.

    Conclusions: We show that the neutron shell effect that governs the existence of the dimolecular states around the third minimum is consistent with the spherical-to-deformed shape transition in the Zr andMo isotopes around N = 58.We demonstrate that the depth of

  4. Third minima in thorium and uranium isotopes in a self-consistent theory

    NASA Astrophysics Data System (ADS)

    McDonnell, J. D.; Nazarewicz, W.; Sheikh, J. A.

    2013-05-01

    Background: Well-developed third minima, corresponding to strongly elongated and reflection-asymmetric shapes associated with dimolecular configurations, have been predicted in some non-self-consistent models to impact fission pathways of thorium and uranium isotopes. These predictions have guided the interpretation of resonances seen experimentally. On the other hand, self-consistent calculations consistently predict very shallow potential-energy surfaces in the third minimum region.Purpose: We investigate the interpretation of third-minimum configurations in terms of dimolecular (cluster) states. We study the isentropic potential-energy surfaces of selected even-even thorium and uranium isotopes at several excitation energies. In order to understand the driving effects behind the presence of third minima, we study the interplay between pairing and shell effects.Methods: We use the finite-temperature superfluid nuclear density functional theory. We consider two Skyrme energy density functionals: a traditional functional SkM* and a recent functional UNEDF1 optimized for fission studies.Results: We predict very shallow or no third minima in the potential-energy surfaces of 232Th and 232U. In the lighter Th and U isotopes with N=136 and 138, the third minima are better developed. We show that the reflection-asymmetric configurations around the third minimum can be associated with dimolecular states involving the spherical doubly magic 132Sn and a lighter deformed Zr or Mo fragment. The potential-energy surfaces for 228,232Th and 232U at several excitation energies are presented. We also study isotopic chains to demonstrate the evolution of the depth of the third minimum with neutron number.Conclusions: We show that the neutron shell effect that governs the existence of the dimolecular states around the third minimum is consistent with the spherical-to-deformed shape transition in the Zr and Mo isotopes around N=58. We demonstrate that the depth of the third minimum

  5. Isotopic analysis of single uranium and plutonium particles by chemical treatment and mass spectrometry

    NASA Astrophysics Data System (ADS)

    Shinonaga, T.; Esaka, F.; Magara, M.; Klose, D.; Donohue, D.

    2008-11-01

    The isotopic composition of single uranium and plutonium particles was measured with an inductively coupled plasma mass spectrometer (ICP-MS) and a thermal ionization mass spectrometer (TIMS). Particles deposited on a carbon planchet were first analyzed with an energy dispersive X-ray spectrometer (EDX) attached to a scanning electron microscope (SEM) and then transferred on to a silicon wafer using a manipulator. The particle on the silicon wafer was dissolved with nitric acid and the isotopic ratios of U and Pu were measured with ICP-MS and TIMS. The results obtained by both methods for particles of certified reference materials showed good agreement with the certified values within the expected uncertainty. The measurement uncertainties obtained in this study were similar for both mass spectrometric methods. This study was performed to establish the method of particle analysis with SEM, EDX, the particle manipulation and chemical preparation technique, and the measurement of isotopic ratios of U and Pu in a single particle by mass spectrometry.

  6. Isotopic Tracking of Hanford 300 Area Derived Uranium in the Columbia River

    SciTech Connect

    Christensen, John N.; Dresel, P. Evan; Conrad, Mark E.; Patton, Gregory W.; DePaolo, Donald J.

    2010-12-01

    A portion of the subsurface contamination at the Hanford Site, the former plutonium production facility in Washington State, affects the Columbia River. A component of this contamination, uranium (U), has variable isotopic composition due to nuclear industrial processes carried out at the site. This characteristic makes it possible to use high-precision isotopic measurements of U in environmental samples to identify even trace levels of contaminant U, determine its sources, and estimate discharge rates. Our data on river water samples indicate that as much as 3.2 kg/day can enter the Columbia River from the 300 Area of the Hanford Site, which is only a small fraction of the total load of dissolved natural background U carried by the Columbia River. This very low–level contamination can be discerned, despite further dilution to <1% of natural background U, as far as 350 km downstream from the Hanford Site. These results indicate that isotopic methods can allow the amounts of U contamination from the Hanford Site to be measured accurately enough to ascertain where they are an environmental concern, and where they are insignificant.

  7. Isotopic composition ( 238U/ 235U) of some commonly used uranium reference materials

    NASA Astrophysics Data System (ADS)

    Condon, Daniel J.; McLean, Noah; Noble, Stephen R.; Bowring, Samuel A.

    2010-12-01

    We have determined 238U/ 235U ratios for a suite of commonly used natural (CRM 112a, SRM 950a, and HU-1) and synthetic (IRMM 184 and CRM U500) uranium reference materials by thermal ionisation mass-spectrometry (TIMS) using the IRMM 3636 233U- 236U double spike to accurately correct for mass fractionation. Total uncertainty on the 238U/ 235U determinations is estimated to be <0.02% (2σ). These natural 238U/ 235U values are different from the widely used 'consensus' value (137.88), with each standard having lower 238U/ 235U values by up to 0.08%. The 238U/ 235U ratio determined for CRM U500 and IRMM 184 are within error of their certified values; however, the total uncertainty for CRM U500 is substantially reduced (from 0.1% to 0.02%). These reference materials are commonly used to assess mass-spectrometer performance and accuracy, calibrate isotope tracers employed in U, U-Th and U-Pb isotopic studies, and as a reference for terrestrial and meteoritic 238U/ 235U variations. These new 238U/ 235U values will thus provide greater accuracy and reduced uncertainty for a wide variety of isotopic determinations.

  8. Determination of total and isotopic uranium and total thorium in soils by inductively coupled plasma-mass spectrometry

    SciTech Connect

    Bolin, R.N.

    1995-12-31

    Inductively coupled plasma-mass spectrometry (ICP-MS), using standard sample introduction by peristaltic pumping, is presented as a method to determine total and isotopic uranium ({sup 234}U, {sup 235}U, {sup 236}U, and {sup 238}U) and thorium ({sup 232}Th) in soil samples. Initial sample preparation consists of oven drying to determine moisture content, and grinding and mixing the soil to make it homogeneous. This is followed by a nitric/hydrofluoric acid digestion to bring the uranium into solution. Bismuth ({sup 209}Bi) is added prior to digestion to monitor for losses due to sample preparation and analysis. An addition digestion, using nitric/perchloric acid is performed if the total thorium concentration is required on the sample. The uranium and thorium content of this solution and the {sup 235}U/{sup 238}U ratio are measured on an initial pass through the ICP-MS. The total uranium measurement is based on the {sup 238}U isotope measurement with correction for the presence of the U isotopes. To determine the concentration of the less abundant {sup 234}U and {sup 236}U isotopes, the digestate is further concentrated by using a solid phase extraction column (TRU.Spec by EiChrom Industries, Inc.) before a second pass through the ICP-MS.

  9. Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia

    NASA Astrophysics Data System (ADS)

    Tissot, François L. H.; Dauphas, Nicolas

    2015-10-01

    The 238U/235U isotopic composition of uranium in seawater can provide important insights into the modern U budget of the oceans. Using the double spike technique and a new data reduction method, we analyzed an array of seawater samples and 41 geostandards covering a broad range of geological settings relevant to low and high temperature geochemistry. Analyses of 18 seawater samples from geographically diverse sites from the Atlantic and Pacific oceans, Mediterranean Sea, Gulf of Mexico, Persian Gulf, and English Channel, together with literature data (n = 17), yield a δ238U value for modern seawater of -0.392 ± 0.005‰ relative to CRM-112a. Measurements of the uranium isotopic compositions of river water, lake water, evaporites, modern coral, shales, and various igneous rocks (n = 64), together with compilations of literature data (n = 380), allow us to estimate the uranium isotopic compositions of the various reservoirs involved in the modern oceanic uranium budget, as well as the fractionation factors associated with U incorporation into those reservoirs. Because the incorporation of U into anoxic/euxinic sediments is accompanied by large isotopic fractionation (ΔAnoxic/Euxinic-SW = +0.6‰), the size of the anoxic/euxinic sink strongly influences the δ238U value of seawater. Keeping all other fluxes constant, the flux of uranium in the anoxic/euxinic sink is constrained to be 7.0 ± 3.1 Mmol/yr (or 14 ± 3% of the total flux out of the ocean). This translates into an areal extent of anoxia into the modern ocean of 0.21 ± 0.09% of the total seafloor. This agrees with independent estimates and rules out a recent uranium budget estimate by Henderson and Anderson (2003). Using the mass fractions and isotopic compositions of various rock types in Earth's crust, we further calculate an average δ238U isotopic composition for the continental crust of -0.29 ± 0.03‰ corresponding to a 238U/235U isotopic ratio of 137.797 ± 0.005. We discuss the implications of

  10. The uranium isotopic composition of the Earth and the Solar System

    NASA Astrophysics Data System (ADS)

    Goldmann, Alexander; Brennecka, Gregory; Noordmann, Janine; Weyer, Stefan; Wadhwa, Meenakshi

    2015-01-01

    Recent high-precision mass spectrometric studies of the uranium isotopic composition of terrestrial and meteoritic materials have shown significant variation in the 238U/235U ratio, which was previously assumed to be invariant (=137.88). In this study, we have investigated 27 bulk meteorite samples from different meteorite groups and types, including carbonaceous (CM1 and CV3), enstatite (EH4) and ordinary (H-, L-, and LL-) chondrites, as well as a variety of achondrites (angrites, eucrites, and ungrouped) to constrain the distribution of U isotopic heterogeneities and to determine the average 238U/235U for the Solar System. The investigated bulk meteorites show a range in 238U/235U between 137.711 and 137.891 (1.3‰) with the largest variations among ordinary chondrites (OCs). However, the U isotope compositions of 20 of the 27 meteorites analyzed here overlap within analytical uncertainties with the narrow range defined by terrestrial basalts (137.778-137.803), which are likely the best representatives for the U isotope composition of the bulk silicate Earth. Furthermore, the average 238U/235U of all investigated meteorite groups overlaps with that of terrestrial basalts (137.795 ± 0.013). The bulk meteorite samples studied here do not show a negative correlation of 238U/235U with Nd/U or Th/U (used as proxies for the Cm/U ratio), as would be expected if radiogenic 235U was generated by the decay of extant 247Cm in the early Solar System. Rather, ordinary chondrites show a positive correlation of 238U/235U with Nd/U and with 1/U. The following conclusions can be drawn from this study: (1) The Solar System has a broadly homogeneous U isotope composition, and bulk samples of only a limited number of meteorites display detectable U isotope variations; (2) Bulk planetary differentiation has no significant effect on the 238U/235U ratio since the Earth, achondrites, and chondrites have indistinguishable U isotope compositions in average. (3) The cause of U isotopic

  11. Uranium isotopic data in uraninite spent fuel from the Bangombe natural nuclear reactor (Gabon) and its surroundings

    PubMed

    Fernandez-Diaz; Quejido; Crespo; Perez del Villar L; Martin-Sanchez; Lozano

    2000-07-01

    In the framework of the "Oklo-Natural Analogue Phase II" Project, uraninite from the Bangombe natural reactor and samples from its host rock were analyzed to determine their uranium isotopic composition by thermal ionisation mass spectrometry, inductively coupled plasma mass spectrometry and alpha spectrometry. There were several objectives for this work: (i) to validate the 235U/238U isotopic ratios obtained by these techniques; (ii) to test the use of the 235U/238U ratio of uraninite as a tracer of migration/retention processes of uranium from the source term to the far field; (iii) to evaluate the most recent migration/retention processes of uranium in the system by U-series disequilibrium. PMID:10879844

  12. Age of uranium mineralization at the Jabiluka and Ranger deposits, Northern Territory, Australia: New U- Pb isotope evidence.

    USGS Publications Warehouse

    Ludwig, K. R.; Grauch, R.I.; Nutt, C.J.; Nash, J.T.; Frishman, D.; Simmons, K.R.

    1987-01-01

    The Ranger and Jabiluka uranium deposits are the largest in the Alligator Rivers uranium field, which contains at least 20% of the world's low-cost uranium reserves. Ore occurs in early Proterozoic metasediments, below an unconformity with sandstones of the 1.65 b.y.-old Kombolgie Formation. This study has used U-Pb isotope data from a large number of whole-rock drill core samples with a variety of mineral assemblages and textures. Both Ranger and Jabiluka reflect a common, profound isotopic disturbance at about 400 to 600 m.y. This disturbance, which was especially pronounced at Jabiluka, may correspond to the development of basins and associated basalt flows to the W and SW.-from Authors

  13. Experimental investigation of uranium-series isotope mobility in a basaltic weathering profile

    NASA Astrophysics Data System (ADS)

    Dosseto, Anthony; Menozzi, Davide; Kinsley, Leslie

    2015-04-01

    The measurement of uranium (U)-series isotopes in regolith can be used to determine the formation rate of weathering profiles. This approach aims at following how the U-series isotope composition of primary minerals (i.e. those derived from the parent material) vary during the development of the weathering profile. Nevertheless, regolith samples are a complex mixture of primary minerals, secondary minerals that are the residue of primary mineral weathering, secondary minerals that precipitate from pore water, minerals derived from atmospheric deposition and organic matter. In this study, firstly we aim at isolating primary minerals and the secondary minerals derived from them, by evaluating a sequential extraction procedure designed to eliminate carbonates, Fe-Mn oxides and organic matter. Secondly, we investigate the behaviour of U-series isotopes during primary mineral dissolution by applying a mild HF/HCl etching solution to the residues of the sequential extraction. These experiments were performed on bedrock, saprolite and soil derived from a basaltic weathering profile in south-eastern Australia. Results show that up to 50% of U is removed during sequential extraction, suggesting that (i) there is a large pool of labile U in the bedrock and (ii) secondary phases and organic matter account for a large fraction of the U budget in bulk saprolite and soil. Sequential extraction has little impact on the (234U/238U) activity ratio of bedrock and saprolite, whilst it shows a decrease in soil. This suggests that the pool of U removed from bedrock and saprolite has a (234U/238U) similar to that of primary minerals; but in the soil, the U removed (mostly from organic matter) is enriched in 234U. This is expected as organic matter uptakes U from pore solutions, which are generally enriched in 234U. During HF/HCl etching, the (234U/238U) of bedrock and saprolite is greater than 1. Sheng and Kuroda [1] previously proposed that (234U/238U) >1 in rocks could be explained by

  14. Application of Inductively Coupled Plasma Mass Spectrometry to the determination of uranium isotope ratios in individual particles for nuclear safeguards

    NASA Astrophysics Data System (ADS)

    Zhang, Xiao Zhi; Esaka, Fumitaka; Esaka, Konomi T.; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu; Watanabe, Kazuo

    2007-10-01

    The capability of inductively coupled plasma mass spectrometry (ICP-MS) for the determination of uranium isotope ratios in individual particles was determined. For this purpose, we developed an experimental procedure including single particle transfer with a manipulator, chemical dissolution and isotope ratio analysis, and applied to the analysis of individual uranium particles in certified reference materials (NBL CRM U050 and U350). As the result, the 235U/ 238U isotope ratio for the particle with the diameter between 0.5 and 3.9 μm was successfully determined with the deviation from the certified ratio within 1.8%. The relative standard deviation (R.S.D.) of the 235U/ 238U isotope ratio was within 4.2%. Although the analysis of 234U/ 238U and 236U/ 238U isotope ratios gave the results with inferior precision, the R.S.D. within 20% was possible for the measurement of the particle with the diameter more than 2.1 μm. The developed procedure was successfully applied to the analysis of a simulated environmental sample prepared from a mixture of indoor dust (NIST SRM 2583) and uranium particles (NBL CRM U050, U350 and U950a). From the results, the proposed procedure was found to be an alternative analytical tool for nuclear safeguards.

  15. Fuel Grading Study on a Low-Enriched Uranium Fuel Design for the High Flux Isotope Reactor

    SciTech Connect

    Ilas, Germina; Primm, Trent

    2009-11-01

    An engineering design study that would enable the conversion of the High Flux Isotope Reactor (HFIR) from high-enriched uranium to low-enriched uranium fuel is ongoing at Oak Ridge National Laboratory. The computational models used to search for a low-enriched uranium (LEU) fuel design that would meet the requirements for the conversion study, and the recent results obtained with these models during FY 2009, are documented and discussed in this report. Estimates of relevant reactor performance parameters for the LEU fuel core are presented and compared with the corresponding data for the currently operating high-enriched uranium fuel core. These studies indicate that the LEU fuel design would maintain the current performance of the HFIR with respect to the neutron flux to the central target region, reflector, and beam tube locations.

  16. Design Study for a Low-Enriched Uranium Core for the High Flux Isotope Reactor, Annual Report for FY 2008

    SciTech Connect

    Primm, Trent; Chandler, David; Ilas, Germina; Miller, James Henry; Sease, John D; Jolly, Brian C

    2009-03-01

    This report documents progress made during FY 2008 in studies of converting the High Flux Isotope Reactor (HFIR) from highly 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 alloy. With axial and radial grading 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 reactor performance from the current level. Results of selected benchmark studies imply that calculations of LEU performance are accurate. Scoping experiments with various manufacturing methods for forming the LEU alloy profile are presented.

  17. Applications with Near-Barrier Photo-Fission Reactions in Uranium Isotopes

    NASA Astrophysics Data System (ADS)

    Johnson, M. S.; Hall, J. M.; McNabb, D. P.; Tuffley, M. J.; Ahmed, M. W.; Stave, S.; Weller, H. R.; Karwowski, H. J.; Tompkins, J. R.

    2010-11-01

    Homeland security programs are developing compact, linearly polarized, quasi-monoenergetic photon sources to probe containers for special nuclear material (SNM). These sources are important in national security applications within the commerce system because of the low dose compared to current bremsstrahlung-based sources used for radiography, and important safety concern. Basic radiography only offers density distributions in cargo containers and does not distinguish fissionable materials from non-fissionable, high-Z materials. One possible usage of quasi-monoenergetic sources is to look for photo-neutrons, which may be subject to lower backgrounds, especially near the barrier where photo-fission neutrons have a high energy tail relative to (g,n). For this presentation, we discuss the results of recent near-barrier photo-fission resonance measurements in uranium isotopes. We will present our study of the neutron data and discuss its viability as a signature for SNM detection applications.

  18. On the accuracy of gamma spectrometric isotope ratio measurements of uranium

    NASA Astrophysics Data System (ADS)

    Ramebäck, H.; Lagerkvist, P.; Holmgren, S.; Jonsson, S.; Sandström, B.; Tovedal, A.; Vesterlund, A.; Vidmar, T.; Kastlander, J.

    2016-04-01

    The isotopic composition of uranium was measured using high resolution gamma spectrometry. Two acid solutions and two samples in the form of UO2 pellets were measured. The measurements were done in close geometries, i.e. directly on the endcap of the high purity germanium detector (HPGe). Applying no corrections for count losses due to true coincidence summing (TCS) resulted in up to about 40% deviation in the abundance of 235U from the results obtained with mass spectrometry. However, after correction for TCS, excellent agreement was achieved between the results obtained using two different measurement methods, or a certified value. Moreover, after corrections, the fitted relative response curves correlated excellently with simulated responses, for the different geometries, of the HPGe detector.

  19. Comparison of the isotopic abundance of U235 and U238 and the radium activity ratios in Colorado Plateau uranium ores

    USGS Publications Warehouse

    Senftle, F.E.; Stieff, L.; Cuttitta, F.; Kuroda, P.K.

    1957-01-01

    The isotopic abundances of uranium and the radium activity ratios of eleven samples of uranium ore from the Colorado Plateau have been measured. No significant variation in the isotopic abundance of the uranium was noted; with'in the experimental error, the average U235/U238 ratio is 137.7. There is a significant variation in the Ra226/Ra223 activity ratios (0.048-0.143), which indicates a relatively recent alteration of the ore samples. The variations do not, however, explain the lead-uranium and lead-lead age discrepancies. ?? 1957.

  20. A new ground-level fallout record of uranium and plutonium isotopes for northern temperate latitudes

    NASA Astrophysics Data System (ADS)

    Warneke, Thorsten; Croudace, Ian W.; Warwick, Phillip E.; Taylor, Rex N.

    2002-11-01

    Plutonium and uranium isotope ratios can be used to differentiate the sources of nuclear contamination from nuclear weapon establishments (Environ. Sci. Technol. 34 (2000) 4496; Internal Report for AWRE Aldermaston, UK (1961)), weapon fallout (Geochim. Cosmochim. Acta 51 (1987) 2623; Earth Planet. Sci. Lett. 63 (1983) 202; Earth Planet. Sci. Lett. 22 (1974) 111; Geochim. Cosmochim. Acta 64 (2000) 989), reprocessing plants, reactor or satellite accidents (Science 105 (1979) 583; Science 238 (1987) 512) and in addition they provide markers for post-1952 geochronology of environmental systems. A good record of plutonium and uranium isotope ratios of the background resulting from atmospheric nuclear testing is essential for source characterisation studies. Using recently developed mass spectrometric techniques (J. Anal. At. Spectrom. 16 (2001) 279) we present here the first complete records between 1952 and the present day of northern temperate latitude 240Pu/ 239Pu and 238U/ 235U atom ratios for atmospheric deposition. Such information was not derived directly during the period of atmospheric testing because suitable mass spectrometric capability was not available. The currently derived records are based on an annual herbage archive and a core from an Alpine glacier. These studies reveal hitherto unseen fluctuations in the 238U/ 235U atmospheric fallout record, some of which are directly related to nuclear testing. In addition, they also provide the first evidence that plutonium contamination originating from Nevada Desert atmospheric weapon tests in 1952 and 1953 extended eastwards as far as northwestern Europe. The results presented here demonstrate that we now have the capability to detect and precisely identify sources of plutonium in the environment with implications for the development of atmospheric transport models, recent geochronology and environmental studies.

  1. Innovative lasers for uranium isotope separation. Final report, September 1, 1989--April 1, 1993

    SciTech Connect

    Brake, M.L.; Gilgenbach, R.M.

    1993-07-01

    Copper vapor laser have important applications to uranium atomic vapor laser isotope separation (AVLIS). We have investigated two innovative methods of exciting/pumping copper vapor lasers which have the potential to improve the efficiency and scaling of large laser systems used in uranium isotope separation. Experimental research has focused on the laser discharge kinetics of (1) microwave, and (2) electron beam excitation/pumping of large-volume copper vapor lasers. Microwave resonant cavity produced copper vapor plasmas at 2.45 GHz, have been investigated in three separate experimental configurations. The first examined the application of CW (0-500W) power and was found to be an excellent method for producing an atomic copper vapor from copper chloride. The second used a pulsed (5kW, 0.5--5 kHz) signal superimposed on the CW signal to attempt to produce vaporization, dissociation and excitation to the laser states. Enhanced emission of the optical radiation was observed but power densities were found to be too low to achieve lasing. In a third experiment we attempted to increase the applied power by using a high power magnetron to produce 100 kW of pulsed power. Unfortunately, difficulties with the magnetron power supply were encountered leaving inconclusive results. Detailed modeling of the electromagnetics of the system were found to match the diagnostics results well. An electron beam pumped copper vapor system (350 kV, 1.0 kA, 300 ns) was investigated in three separate copper chloride heating systems, external chamber, externally heated chamber and an internally heated chamber. Since atomic copper spectral lines were not observed, it is assumed that a single pulse accelerator is not capable of both dissociating the copper chloride and exciting atomic copper and a repetitively pulsed electron beam generator is needed.

  2. On monitoring anthropogenic airborne uranium concentrations and (235)U/(238)U isotopic ratio by Lichen - bio-indicator technique.

    PubMed

    Golubev, A V; Golubeva, V N; Krylov, N G; Kuznetsova, V F; Mavrin, S V; Aleinikov, A Yu; Hoppes, W G; Surano, K A

    2005-01-01

    Lichens are widely used to assess the atmospheric pollution by heavy metals and radionuclides. However, few studies are available in publications on using lichens to qualitatively assess the atmospheric pollution levels. The paper presents research results applying epiphytic lichens as bio-monitors of quantitative atmospheric contamination with uranium. The observations were conducted during 2.5 years in the natural environment. Two experimental sites were used: one in the vicinity of a uranium contamination source, the other one - at a sufficient distance away to represent the background conditions. Air and lichens were sampled at both sites monthly. Epiphytic lichens Hypogimnia physodes were used as bio-indicators. Lichen samples were taken from various trees at about 1.5m from the ground. Air was sampled with filters at sampling stations. The uranium content in lichen and air samples as well as isotopic mass ratios (235)U/(238)U were measured by mass-spectrometer technique after uranium pre-extraction. Measured content of uranium were 1.45 mgkg(-1) in lichen at 2.09 E-04 microgm(-3) in air and 0.106 mgkg(-1) in lichen at 1.13 E-05 microgm(-3) in air. The relationship of the uranium content in atmosphere and that in lichens was determined, C(AIR)=exp(1.1 x C(LICHEN)-12). The possibility of separate identification of natural and man-made uranium in lichens was demonstrated in principle. PMID:16083999

  3. A Metal Stable Isotope Approach to Understanding Uranium Mobility Across Roll Front Redox Boundaries

    NASA Astrophysics Data System (ADS)

    Brown, S. T.; Basu, A.; Christensen, J. N.; DePaolo, D. J.; Heikoop, J. M.; Reimus, P. W.; Maher, K.; Weaver, K. L.

    2015-12-01

    Sedimentary roll-front uranium (U) ore deposits are the principal source of U for nuclear fuel in the USA and an important part of the current all-of-the-above energy strategy. Mining of roll-front U ore in the USA is primarily by in situ alkaline oxidative dissolution of U minerals. There are significant environmental benefits to in situ mining including no mine tailings or radioactive dust, however, the long-term immobilization of U in the aquifer after the completion of mining remains uncertain. We have utilized the metal stable isotopes U, Se and Mo in groundwater from roll-front mines in Texas and Wyoming to quantify the aquifer redox conditions and predict the onset of U reduction after post mining aquifer restoration. Supporting information from the geochemistry of groundwater and aquifer sediments are used to understand the transport of U prior to and after in situ mining. Groundwater was collected across 4 mining units at the Rosita mine in the Texas coastal plain and 2 mining units at the Smith Ranch mine in the Powder River Basin, Wyoming. In general, the sampled waters are moderately reducing and ore zone wells contain the highest aqueous U concentrations. The lowest U concentrations occur in monitoring wells downgradient of the ore zone. 238U/235U is lowest in downgradient wells and is correlated with aqueous U concentrations. Rayleigh distillation models of the 238U/235U are consistent with U isotope fractionation factors of 1.0004-1.001, similar to lab-based studies. Based on these results we conclude that redox reactions continue to affect U distribution in the ore zone and downgradient regions. We also measured aqueous selenium isotope (δ82Se) and molybdenum isotope (δ98Mo) compositions in the Rosita groundwater. Se(VI) primarily occurs in the upgradient wells and is absent in most ore zone and downgradient wells. Rayleigh distillation models suggest reduction of Se(VI) along the groundwater flow path and when superimposed on the U isotope data

  4. Performance testing of the upgraded uranium isotopics multi-group analysis code MGAU

    NASA Astrophysics Data System (ADS)

    Berlizov, A. N.; Gunnink, R.; Zsigrai, J.; Nguyen, C. T.; Tryshyn, V. V.

    2007-06-01

    The paper describes recent developments of the MGAU (Multi-Group Analysis for Uranium) method, which resulted in the creation of an upgraded version 4.0 of the MGAU code. The major improvements concerned the procedure of the intrinsic efficiency calibration, particularly in the 120-205 keV region. The results of the tests carried out with the use of certified reference uranium isotopic materials SRM 969 and CRM 146 showed a significantly improved performance of the upgraded MGAU code for the accurate characterization of 235U and 234U abundances. The relative systematic biases of the abundances measured were evaluated not to exceed 1% and 3% over the concentration intervals 0.32-93.2 and 0.002-0.98 mass% for 235U and 234U, respectively. The influence of an up to 4-5 mm steel equivalent absorber and sample thickness on the measurement results was found to be much smaller than in previous versions of the code.

  5. Sulfur isotopes as indicators of amended bacterial sulfate reduction processes influencing field scale uranium bioremediation.

    PubMed

    Druhan, Jennifer L; Conrad, Mark E; Williams, Kenneth H; N'Guessan, Lucie; Long, Philip E; Hubbard, Susan S

    2008-11-01

    Aqueous uranium (U(VI)) concentrations in a contaminated aquifer in Rifle Colorado have been successfully lowered through electron donor amended bioreduction. Samples collected during the acetate amendment experiment were analyzed for aqueous concentrations of Fe(ll), sulfate, sulfide, acetate, U(VI), and delta(34)S of sulfate and sulfide to explore the utility of sulfur isotopes as indicators of in situ acetate amended sulfate and uranium bioreduction processes. Enrichment of up to 7% per hundred in delta(34)S of sulfate in down-gradient monitoring wells indicates a transition to elevated bacterial sulfate reduction. A depletion in Fe(II), sulfate, and sulfide concentrations atthe height of sulfate reduction, along with an increase in the delta(34)S of sulfide to levels approaching the delta(34)S values of sulfate, indicates sulfate limited conditions concurrent with a rebound in U(VI) concentrations. Upon cessation of acetate amendment, sulfate and sulfide concentrations increased, while delta(34)S values of sulfide returned to less than -20% per hundred and sulfate delta(34)S decreased to near-background values, indicating lower levels of sulfate reduction accompanied by a corresponding drop in U(VI). Results indicate a transition between electron donor and sulfate-limited conditions at the height of sulfate reduction and suggest stability of biogenic FeS precipitates following the end of acetate amendment. PMID:19031870

  6. Depleted uranium mobility across a weapons testing site: isotopic investigation of porewater, earthworms, and soils.

    PubMed

    Oliver, Ian W; Graham, Margaret C; MacKenzie, Angus B; Ellam, Robert M; Farmer, John G

    2008-12-15

    The mobility and bioavailability of depleted uranium (DU) in soils at a UK Ministry of Defence (UK MoD) weapons testing range were investigated. Soil and vegetation were collected near a test-firing position and at eight points along a transect line extending approximately 200 m down-slope, perpendicular to the firing line, toward a small stream. Earthworms and porewaters were subsequently separated from the soils and both total filtered porewater (<0.2 microm) and discrete size fractions (0.2 microm-100 kDa, 100-30 kDa, 30-3 kDa, and <3 kDa)obtainedvia centrifugal ultrafiltration were examined. Uranium concentrations were determined by inductively coupled plasma optical emission spectrometry (ICP-OES) for soils and ICP-mass spectrometry (MS) for earthworms and porewaters, while 235U:238U atom ratios were determined by multicollector (MC)-ICP-MS. Comparison of the porewater and earthworm isotopic values with those of the soil solids indicated that DU released into the environment during weapons test-firing operations was more labile and more bioavailable than naturally occurring U in the soils at the testing range. Importantly, DU was shown to be present in soil porewater even at a distance of approximately 185 m from the test-firing position and, along the extent of the transect was apparently associated with organic colloids. PMID:19174886

  7. Sulfur Isotopes as Indicators of Amended Bacterial Sulfate Reduction Processes Influencing Field Scale Uranium Bioremediation

    SciTech Connect

    Druhan, Jennifer L.; Conrad, Mark E.; Williams, Kenneth H.; N'Guessan, A. Lucie; Long, Philip E.; Hubbard, Susan S.

    2008-11-01

    Aqueous uranium (U(VI)) concentrations in a contaminated aquifer in Rifle Colorado have been successfully lowered through electron donor amended bioreduction. Samples collected during the acetate amendment experiment were analyzed for aqueous concentrations of Fe(II), sulfate, sulfide, acetate, U(VI), and δ34S of sulfate and sulfide to explore the utility of sulfur isotopes as indicators of in situ acetate amended sulfate and uranium bioreduction processes. Enrichment of up to 7‰ in δ34S of sulfate in down-gradient monitoring wells indicates a transition to elevated bacterial sulfate reduction. A depletion in Fe(II), sulfate, and sulfide concentrations at the height of sulfate reduction, along with an increase in the δ34S of sulfide to levels approaching the d34S values of sulfate, indicates sulfate limited conditions concurrent with a rebound in U(VI) concentrations. Upon cessation of acetate amendment, sulfate and sulfide concentrations increased, while δ34S values of sulfide returned to less than -20‰ and sulfate δ34S decreased to near-background values, indicating lower levels of sulfate reduction accompanied by a corresponding drop in U(VI). Results indicate a transition between electron donor and sulfate-limited conditions at the height of sulfate reduction and suggest stability of biogenic FeS precipitates following the end of acetate amendment.

  8. Uranium and minor-element partitioning in Fe-Ti oxides and zircon from partially melted granodiorite, Crater Lake, Oregon

    USGS Publications Warehouse

    Tourrette, T.Z.L.; Burnett, D.S.; Bacon, C.R.

    1991-01-01

    Crystal-liquid partitioning in Fe-Ti oxides and zircon was studied in partially melted granodiorite blocks ejected during the climactic eruption of Mt. Mazama (Crater Lake), Oregon. The blocks, which contain up to 33% rhyolite glass (75 wt% SiO2), are interpreted to be portions of the magma chamber walls that were torn off during eruption. The glass is clear and well homogenized for all measured elements except Zr. Results for Fe-Ti oxides give DUoxide/liq ??? 0.1. Partitioning of Mg, Mn, Al, Si, V, and Cr in Fe-Ti oxides indicates that grains surrounded by glass are moderately well equilibrated with the melt for many of the minor elements, while those that are inclusions in relict plagioclase are not. Uranium and ytterbium inhomogeneities in zircons indicate that the zircons have only partially equilibrated with the melt and that uranium appears to have been diffusing out of the zircons faster than the zircons were dissolving. Minimum U, Y, and P concentrations in zircons give maximum DUzrc/liq = 13,DYzrc/liq = 23, and DPzrc/liq = 1, but these are considerably lower than reported by other workers for U and Y. Based on our measurements and given their low abundances in most rocks, Fe-Ti oxides probably do not play a major role in U-Th fractionation during partial melting. The partial melts were undersaturated with zircon and apatite, but both phases are present in our samples. This demonstrates an actual case of non-equilibrium source retention of accessory phases, which in general could be an important trace-element fractionation mechanism. Our results do not support the hypothesis that liquid structure is the dominant factor controlling trace-element partitioning in high-silica rhyolites. Rough calculations based on Zr gradients in the glass indicate that the samples could have been partially molten for 800 to 8000 years. ?? 1991.

  9. Uranium Isotope Evidence for Temporary Ocean Oxygenation Following the Sturtian Glaciation

    NASA Astrophysics Data System (ADS)

    Lau, K. V.; Maher, K.; Macdonald, F. A.; Payne, J.

    2015-12-01

    The link between widespread ocean oxygenation in the Neoproterozoic and the rise of animals has long been debated, largely because the timing and nature of oxygenation of the oceans remain poorly constrained. Strata deposited during the Cryogenian non-glacial interlude (660 to 635 Ma), between the Sturtian and Marinoan Snowball Earth glaciations, contain the earliest fossil evidence of animals. To quantitatively estimate patterns of seafloor oxygenation during this critical interval, we present uranium isotope (δ238U) data from limestone of the Taishir Formation (Fm) in Mongolia in two stratigraphic sections that are separated by ~75 km across the basin. The Taishir Fm hosts two large δ13C excursions that co-vary in total organic and inorganic (carbonate) carbon: a basal carbonate δ13C excursion to -4‰ in the Sturtian cap carbonate, followed by a rise to enriched values of +8‰, a second negative δ13C excursion to -7‰ referred to as the Taishir excursion, followed by a second rise to +10‰. Above the Sturtian glacial deposits, in the stratigraphic interval below the Taishir excursion, δ238U compositions have a mean value that is similar to that of modern seawater. After the Taishir excursion, the δ238U record exhibits a step decrease of ~0.3‰, and δ238U remains approximately constant until the erosional unconformity at the base of the Marinoan glacial deposits. We use a box model to constrain the uranium cycle behavior that best explains our observations. In the model, the best explanation for the less negative post-Sturtian values of δ238U is extensive oxygenation of the seafloor. Moreover, the model demonstrates that the higher δ238U values of the post-Sturtian limestones are inconsistent with an increased flux of uranium to the oceans due to post-Snowball weathering as the primary driver of the excursion. Thus, we favor a scenario in which there was a rise in oxygen levels following the Sturtian glaciation followed by a decrease in seafloor

  10. Optimized Chemical Separation and Measurement by TE TIMS Using Carburized Filaments for Uranium Isotope Ratio Measurements Applied to Plutonium Chronometry.

    PubMed

    Sturm, Monika; Richter, Stephan; Aregbe, Yetunde; Wellum, Roger; Prohaska, Thomas

    2016-06-21

    An optimized method is described for U/Pu separation and subsequent measurement of the amount contents of uranium isotopes by total evaporation (TE) TIMS with a double filament setup combined with filament carburization for age determination of plutonium samples. The use of carburized filaments improved the signal behavior for total evaporation TIMS measurements of uranium. Elevated uranium ion formation by passive heating during rhenium signal optimization at the start of the total evaporation measurement procedure was found to be a result from byproducts of the separation procedure deposited on the filament. This was avoided using carburized filaments. Hence, loss of sample before the actual TE data acquisition was prevented, and automated measurement sequences could be accomplished. Furthermore, separation of residual plutonium in the separated uranium fraction was achieved directly on the filament by use of the carburized filaments. Although the analytical approach was originally tailored to achieve reliable results only for the (238)Pu/(234)U, (239)Pu/(235)U, and (240)Pu/(236)U chronometers, the optimization of the procedure additionally allowed the use of the (242)Pu/(238)U isotope amount ratio as a highly sensitive indicator for residual uranium present in the sample, which is not of radiogenic origin. The sample preparation method described in this article has been successfully applied for the age determination of CRM NBS 947 and other sulfate and oxide plutonium samples. PMID:27240571

  11. The Effect of Redox Mechanisms on the Fractionation of Uranium `Stable' Isotopes

    NASA Astrophysics Data System (ADS)

    Kaltenbach, A.; Stirling, C. H.; Porcelli, D.; Hilton, D. R.; Kulongoski, J. T.

    2010-12-01

    Uranium is the heaviest naturally occurring element. It consists of three natural isotopes, 238U, 235U and 234U and has four oxidation states, U(III)-U(VI), of which only U(IV) and U(VI) are common. In the oxidized, hexavalent condition, U(VI) exists as uranyl ion (UO22+), which forms soluble, non-reactive complexes with carbonates. In the reduced condition, tetravalent U(IV) forms immobile minerals with hydroxides, fluorides and phosphates that are removed from the water column. In the recent years, isotopic fractionation between 235U and 238U has been detected in a range of terrestrial environments. Changes to U concentrations in natural waters occur due to biological uptake, adsorption/desorption to/from particulates and surfaces, diffusion into sediments, and chemically and biologically induced redox mechanisms (Swarzenski et al., 1999, Mar. Chem. 67, 181). The largest isotopic shifts evidently occur during the reduction of U(VI) to U(IV) in waters, during which precipitation changes the dissolved U concentration. However, the exact mechanisms controlling 235U/238U fractionation remain unclear. Some results implicate mass-dependent zero-point energy effects (preferential removal of 235U over 238U) (Rademacher et al., 2006, Environ. Sci. Technol. 40, 6943) as the main cause for the isotopic variations measured, while others suggest volume-dependent nuclear field shift effects (preferential removal of 238U over 235U) (Weyer et al., 2008, GCA 72, 345, Bopp et al., 2010, Environ. Sci. Technol. 44, 5927), which are predicted to be of the opposite sign and up to three times larger than mass-dependent effects. In this study, profiles of two different water masses were examined for their uranium concentration and their 235U/238U isotopic composition to determine the magnitude of the natural isotopic shifts as well as their origins. One set of samples was collected from a 160 m depth profile in the Framvaren Fjord, an anoxic basin. In this basin, the biogeochemical

  12. Uranium isotopes distinguish two geochemically distinct stages during the later Cambrian SPICE event

    PubMed Central

    Dahl, Tais W.; Boyle, Richard A.; Canfield, Donald E.; Connelly, James N.; Gill, Benjamin C.; Lenton, Timothy M.; Bizzarro, Martin

    2015-01-01

    Anoxic marine zones were common in early Paleozoic oceans (542–400 Ma), and present a potential link to atmospheric pO2 via feedbacks linking global marine phosphorous recycling, primary production and organic carbon burial. Uranium (U) isotopes in carbonate rocks track the extent of ocean anoxia, whereas carbon (C) and sulfur (S) isotopes track the burial of organic carbon and pyrite sulfur (primary long-term sources of atmospheric oxygen). In combination, these proxies therefore reveal the comparative dynamics of ocean anoxia and oxygen liberation to the atmosphere over million-year time scales. Here we report high-precision uranium isotopic data in marine carbonates deposited during the Late Cambrian ‘SPICE’ event, at ca. 499 Ma, documenting a well-defined −0.18‰ negative δ238U excursion that occurs at the onset of the SPICE event’s positive δ13C and δ34S excursions, but peaks (and tails off) before them. Dynamic modelling shows that the different response of the U reservoir cannot be attributed solely to differences in residence times or reservoir sizes - suggesting that two chemically distinct ocean states occurred within the SPICE event. The first ocean stage involved a global expansion of euxinic waters, triggering the spike in U burial, and peaking in conjunction with a well-known trilobite extinction event. During the second stage widespread euxinia waned, causing U removal to tail off, but enhanced organic carbon and pyrite burial continued, coinciding with evidence for severe sulfate depletion in the oceans (Gill et al., 2011). We discuss scenarios for how an interval of elevated pyrite and organic carbon burial could have been sustained without widespread euxinia in the water column (both non-sulfidic anoxia and/or a more oxygenated ocean state are possibilities). Either way, the SPICE event encompasses two different stages of elevated organic carbon and pyrite burial maintained by high nutrient fluxes to the ocean, and potentially

  13. Determination of the origin of elevated uranium at a Former Air Force Landfill using non-parametric statistics analysis and uranium isotope ratio analysis

    SciTech Connect

    Weismann, J.; Young, C.; Masciulli, S.; Caputo, D.

    2007-07-01

    factors so that gross alpha action levels can be applied to future long-term landfill monitoring to track radiological conditions at lower cost. Ratios of isotopic uranium results were calculated to test whether the elevated uranium displayed signatures indicative of military use. Results of all ratio testing strongly supports the conclusion that the uranium found in groundwater, surface water, and sediment at OU 2 is naturally-occurring and has not undergone anthropogenic enrichment or processing. U-234:U-238 ratios also show that a disequilibrium state, i.e., ratio greater than 1, exists throughout OU 2 which is indicative of long-term aqueous transport in aged aquifers. These results all support the conclusion that the elevated uranium observed at OU 2 is due to the high concentrations in the regional watershed. Based on the results of this monitoring program, we concluded that the elevated uranium concentrations measured in OU 2 groundwater, surface water, and sediment are due to the naturally-occurring uranium content of the regional watershed and are not the result of waste burials in the former landfill. Several lines of evidence indicate that natural uranium has been naturally concentrated beneath OU 2 in the geologic past and the higher of uranium concentrations in down-gradient wells is the result of geochemical processes and not the result of a uranium ore disposal. These results therefore provide the data necessary to support radiological closure of OU 2. (authors)

  14. PREPARING THE HIGH FLUX ISOTOPE REACTOR FOR CONVERSION TO LOW ENRICHED URANIUM FUEL ? RETURN TO 100 MW

    SciTech Connect

    Smith, Kevin Arthur; Primm, Trent

    2009-01-01

    The feasibility of low-enriched uranium (LEU) fuel as a replacement for the current, high enriched uranium (HEU) fuel for the High Flux Isotope Reactor (HFIR) has been under study since 2006. Reactor performance studies have been completed for conceptual plate designs and show that maintaining reactor performance while converting to LEU fuel requires returning the reactor power to 100 MW from 85 MW. The analyses required to up-rate the reactor power and the methods to perform these analyses are discussed. Comments regarding the regulatory approval process are provided along with a conceptual schedule.

  15. Investigation of the oxygen isotopic composition in oxidic uranium compounds as a new property in nuclear forensic science.

    PubMed

    Pajo, L; Mayer, K; Koch, L

    2001-10-01

    The analysis of seized nuclear material aims at identifying the origin of the material. Determination of the n(18O)/n(16O) ratio for the uranium oxide adds another characteristic property to the pattern which enables location of the production area of the material. A method has been developed for n(18O)/n(16O) ratio measurement which uses thermal ionization mass spectrometric (TIMS) analysis of the 238UO+ species. It has been shown that uranium oxides of different geographic origin have significantly different n(18O)/n(16O) ratios, whereas different samples of the same origin have constant oxygen isotopes ratios. PMID:11688648

  16. Uranium Isotopes in Fine-grained Clastic Sediments: A New Perspective on Erosion and Sedimentation

    NASA Astrophysics Data System (ADS)

    Depaolo, D. J.; Maher, K.; Christensen, J. N.; McManus, J.

    2005-12-01

    High precision uranium isotope measurements may provide a means of determining the timescale associated with the transformation of bedrock to sediment, which includes the time required to mechanically break down rock into transportable fragments, the residence time of sediment particles in soils, streambeds, floodplains, dunes, and moraines, and their transport by wind, rivers and ocean currents to the site of final deposition on the seafloor or in lakes. The interpretation of variations in the 234U/238U ratios in sediments is based on a model for the disruption of the 238U decay series due to the loss of the decay product 234Th by recoil associated with the alpha decay of 238U. This paper presents the results of a study of 234U/238U ratios, as well as O, Nd and Sr isotopes, in fine-grained deep sea sediments, 0 to about 400 ky in age, cored in the North Atlantic Ocean at Ocean Drilling Program Site 984A. The sediments are largely siliciclastic, but have a significant carbonate component that varies between a few and 30 per cent by volume. The O isotope data obtained on separated foraminifera clearly show the last several glacial cycles, and thus provide a detailed temporal framework for the sediments. The Nd and Sr isotopic data show that the provenance of the sediment has oscillated, roughly but not exactly, in concert with the extent of continental ice volume, between a local source - probably volcanic rocks from Iceland - and a continental source. An unexpected finding is that the 234U/238U ratios of the siliciclastic portion of the sediment, isolated by leaching, show large and systematic variations that are correlated with glacial cycles and to some degree with sediment provenance. The U isotope variations are inferred to reflect differences in the transport time of the sediment - the time elapsed between the generation of the small sediment particles on Iceland and the continental source areas, and the time of deposition on the seafloor in the North Atlantic

  17. Isotopic evidence for reductive immobilization of uranium across a roll-front mineral deposit

    DOE PAGESBeta

    Brown, Shaun T.; Basu, Anirban; Christensen, John N.; Reimus, Paul; Heikoop, Jeffrey; Simmons, Ardyth; Woldegabriel, Giday; Maher, Kate; Weaver, Karrie; Clay, James; et al

    2016-06-21

    We use uranium (U) isotope ratios to detect and quantify the extent of natural U reduction in groundwater across a roll front redox gradient. Our study was conducted at the Smith Ranch-Highland in situ recovery (ISR) U mine in eastern Wyoming, USA, where economic U deposits occur in the Paleocene Fort Union formation. To evaluate the fate of aqueous U in and adjacent to the ore body, we investigated the chemical composition and isotope ratios of groundwater samples from the roll-front type ore body and surrounding monitoring wells of a previously mined area. The 238U/235U of groundwater varies by approximatelymore » 3‰ and is correlated with U concentrations. Fluid samples down-gradient of the ore zone are the most depleted in 238U and have the lowest U concentrations. Activity ratios of 234U/238U are ~5.5 up-gradient of the ore zone, ~1.0 in the ore zone, and between 2.3 and 3.7 in the down-gradient monitoring wells. High-precision measurements of 234U/238U and 238U/235U allow for development of a conceptual model that evaluates both the migration of U from the ore body and the extent of natural attenuation due to reduction. We find that the premining migration of U down-gradient of the delineated ore body is minimal along eight transects due to reduction in or adjacent to the ore body, whereas two other transects show little or no sign of reduction in the down-gradient region. Lastly, these results suggest that characterization of U isotopic ratios at the mine planning stage, in conjunction with routine geochemical analyses, can be used to identify where more or less postmining remediation will be necessary.« less

  18. Using Pb isotopes in surface media to distinguish anthropogenic sources from undercover uranium sources

    NASA Astrophysics Data System (ADS)

    Kyser, Kurt; Lahusen, Larry; Drever, Garth; Dunn, Colin; Leduc, Evelyne; Chipley, Don

    2015-09-01

    The response in elemental concentrations and Pb isotopes in various surface media from the Cigar West unconformity-type uranium deposit located at a depth of 450 m were measured to ascertain if element migration from the deposit can be detected at the surface. The media included clay-size fractions separated from the A2, B and C soil horizons, and tree cores and twigs from black spruce (Picea mariana) and jack pine (Pinus banksiana) trees. Lead isotopes were used to trace any effect on the surface media from the deposit at depth because the 207Pb/206Pb ratios in the ore are < 0.1, whereas the background values in the basin are > 0.7 and modern anthropogenic Pb from aerosols are near 0.9. The tree cores record their lowest and therefore most radiogenic 207Pb/206Pb ratios of < 0.7 near the surface projection of the deposit and associated structures, particularly in tree rings that predate any exploration and drilling activity in the area. The median 207Pb/206Pb ratios increase in the order C, B soil horizon clays, tree cores, A2 soil clays and twigs because of the increasing contribution of common Pb with high ratios from anthropogenic sources that affect the shallowest media the most. Although this anthropogenic Pb as well as that from the background dominates the composition of all media at the surface and the contribution from the deposit at depth is diminished toward the surface, ore-related Pb is still present as a few percent of the composition of pathfinder elements and Pb isotopes.

  19. Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit.

    PubMed

    Brown, Shaun T; Basu, Anirban; Christensen, John N; Reimus, Paul; Heikoop, Jeffrey; Simmons, Ardyth; Woldegabriel, Giday; Maher, Kate; Weaver, Karrie; Clay, James; DePaolo, Donald J

    2016-06-21

    We use uranium (U) isotope ratios to detect and quantify the extent of natural U reduction in groundwater across a roll front redox gradient. Our study was conducted at the Smith Ranch-Highland in situ recovery (ISR) U mine in eastern Wyoming, USA, where economic U deposits occur in the Paleocene Fort Union formation. To evaluate the fate of aqueous U in and adjacent to the ore body, we investigated the chemical composition and isotope ratios of groundwater samples from the roll-front type ore body and surrounding monitoring wells of a previously mined area. The (238)U/(235)U of groundwater varies by approximately 3‰ and is correlated with U concentrations. Fluid samples down-gradient of the ore zone are the most depleted in (238)U and have the lowest U concentrations. Activity ratios of (234)U/(238)U are ∼5.5 up-gradient of the ore zone, ∼1.0 in the ore zone, and between 2.3 and 3.7 in the down-gradient monitoring wells. High-precision measurements of (234)U/(238)U and (238)U/(235)U allow for development of a conceptual model that evaluates both the migration of U from the ore body and the extent of natural attenuation due to reduction. We find that the premining migration of U down-gradient of the delineated ore body is minimal along eight transects due to reduction in or adjacent to the ore body, whereas two other transects show little or no sign of reduction in the down-gradient region. These results suggest that characterization of U isotopic ratios at the mine planning stage, in conjunction with routine geochemical analyses, can be used to identify where more or less postmining remediation will be necessary. PMID:27203292

  20. The Behaviour of Uranium and Lithium Isotopes During Basalt Weathering and Erosion

    NASA Astrophysics Data System (ADS)

    Pogge von Strandmann, P. A.; Burton, K. W.; James, R. H.; van Calsteren, P.; Gislason, S.

    2005-12-01

    Basalt weathering rates are higher than for many other silicate rocks, and thus exert a strong control on atmospheric CO2 [1]. Moreover, variations in weathering in response to climatic or tectonic change will inevitably affect chemical fluxes to the oceans. Li isotopes potentially provide key information on weathering rates, but their behaviour in the riverine and estuarine environment remains poorly constrained. While U-series nuclides can give information on both the weathering process and the timescale over which it occurs, comparison of both U and Li provides some insight into the processes which govern the geochemical cycles of each element. This study presents new U and Li isotope data for rivers draining basalt terrains in Iceland and Sao Miguel (Azores). Both of these islands are essentially monolithologic, but have different climatic regimes, and variations in river chemistry are linked to differences in the weathering environment, rather than to rock type. River waters from Iceland were taken from both a large catchment in the west of the island, an associated estuary, and from glacial rivers in the south. The U concentration in the rivers ranges from 0.2 to 20 ng/l, and rises from 3 ng/l to almost 3 μg/l in the estuary, showing conservative behaviour in the mixing zone. Li concentrations range from 0.02 to 1.05 μg/l in the rivers, and rise to 160 μg/l in the estuary. Li also behaves conservatively in the mixing zone. For the Azores U and Li river concentrations range from 3 to 212 ng/l and from 0.09 to 3.5 μg/l, respectively. Highest concentrations are linked to hydrothermal input. Uranium activity ratios (234U/238U) range from 1.13 to 2.14 in Iceland, and from 1.02 to 1.92 in the Azores, showing that silicate weathering can yield a large range of values (down to 1, which is secular equilibrium). Lowest U concentrations typically correspond to highest activity ratios, especially in glacial rivers. The behaviour of U in the catchment shows mixing

  1. Measurement of the isotopic composition of uranium micrometer-size particles by femtosecond laser ablation-inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Hubert, Amélie; Claverie, Fanny; Pécheyran, Christophe; Pointurier, Fabien

    In this paper, we will describe and indicate the performance of a new method based on the use of femtosecond laser ablation (fs-LA) coupled to a quadrupole-based inductively coupled plasma mass spectrometer (ICP-QMS) for analyzing the isotopic composition of micrometer-size uranium particles. The fs-LA device was equipped with a high frequency source (till 10 kHz). We applied this method to 1-2 μm diameter-uranium particles of known isotopic composition and we compared this technique with the two techniques currently used for uranium particle analysis: Secondary Ionization Mass Spectrometry (SIMS) and Fission Track Thermal Ionization Mass Spectrometry (FT-TIMS). By optimizing the experimental conditions, we achieved typical accuracy and reproducibility below 4% on 235U/238U for short transient signals of only 15 s related to 10 to 200 pg of uranium. The detection limit (at the 3 sigma level) was ~ 350 ag for the 235U isotope, meaning that 235U/238U isotope ratios in natural uranium particles of ~ 220 nm diameter can be measured. We also showed that the local contamination resulting from the side deposition of ablation debris at ~ 100 μm from the ablation crater represented only a small percentage of the initial uranium signal of the ablated particle. Despite the use of single collector ICP-MS, we were able to demonstrate that fs-LA-ICP-MS is a promising alternative technique for determining uranium isotopic composition in particle analysis.

  2. Rate equation model of laser induced bias in uranium isotope ratios measured by resonance ionization mass spectrometry

    SciTech Connect

    Isselhardt, B. H.; Prussin, S. G.; Savina, M. R.; Willingham, D. G.; Knight, K. B.; Hutcheon, I. D.

    2015-12-07

    Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process between uranium atoms and potential isobars without the aid of chemical purification and separation. The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of the 235U/238U ratio to decrease laser-induced isotopic fractionation. In application, isotope standards are used to identify and correct bias in measured isotope ratios, but understanding laser-induced bias from first-principles can improve the precision and accuracy of experimental measurements. A rate equation model for predicting the relative ionization probability has been developed to study the effect of variations in laser parameters on the measured isotope ratio. The model uses atomic data and empirical descriptions of laser performance to estimate the laser-induced bias expected in experimental measurements of the 235U/238U ratio. Empirical corrections are also included to account for ionization processes that are difficult to calculate from first principles with the available atomic data. As a result, development of this model has highlighted several important considerations for properly interpreting experimental results.

  3. Rate equation model of laser induced bias in uranium isotope ratios measured by resonance ionization mass spectrometry

    DOE PAGESBeta

    Isselhardt, B. H.; Prussin, S. G.; Savina, M. R.; Willingham, D. G.; Knight, K. B.; Hutcheon, I. D.

    2015-12-07

    Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process between uranium atoms and potential isobars without the aid of chemical purification and separation. The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of the 235U/238U ratio to decrease laser-induced isotopic fractionation. In application, isotope standards are used to identify and correct bias in measured isotope ratios, but understanding laser-induced bias from first-principles can improve the precision and accuracy of experimental measurements. A rate equationmore » model for predicting the relative ionization probability has been developed to study the effect of variations in laser parameters on the measured isotope ratio. The model uses atomic data and empirical descriptions of laser performance to estimate the laser-induced bias expected in experimental measurements of the 235U/238U ratio. Empirical corrections are also included to account for ionization processes that are difficult to calculate from first principles with the available atomic data. As a result, development of this model has highlighted several important considerations for properly interpreting experimental results.« less

  4. Validation of Electrochemically Modulated Separations Performed On-Line with MC-ICP-MS for Uranium and Plutonium Isotopic Analyses

    SciTech Connect

    Liezers, Martin; Olsen, Khris B.; Mitroshkov, Alexandre V.; Duckworth, Douglas C.

    2010-08-11

    The most time consuming process in uranium or plutonium isotopic analyses is performing the requisite chromatographic separation of the actinides. Filament preparation for thermal ionization (TIMS) adds further delays, but is generally accepted due to the unmatched performance in trace isotopic analyses. Advances in Multi-Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICP-MS) are beginning to rival the performance of TIMS. Methods, such as Electrochemically Modulated Separations (EMS) can efficiently pre-concentrate U or Pu quite selectively from small solution volumes in a matrix of 0.5 M nitric acid. When performed in-line with ICP-MS, the rapid analyte release from the electrode is fast, and large transient analyte signal enhancements of >100 fold can be achieved as compared to more conventional continuous nebulization of the original starting solution. This makes the approach ideal for very low level isotope ratio measurements. In this paper, some aspects of EMS performance are described. These include low level Pu isotope ratio behavior versus concentration by MC-ICP-MS and uranium rejection characteristics that are also important for reliable low level Pu isotope ratio determinations.

  5. Constrains on the Uranium Isotopic Composition of Seawater and Implications for Coral U/Th Geochronology

    NASA Astrophysics Data System (ADS)

    Chutcharavan, P. M.; Dutton, A.; Ellwood, M. J.

    2015-12-01

    Coral U-series geochronology is an important tool for calibrating records of sea level change during the late Quaternary and coral 14C dates for the radiocarbon timescale. However, coralline aragonite is highly susceptible to diagenesis, and samples must be carefully screened to ensure a specimen is unaltered. One method used to accept or reject U-series ages is the initial coral 234U/238U activity ratio, which reflects the 234U/238U activity of seawater at the time of coral skeleton formation. Due to the long residence time of uranium in the ocean (~400,000 years), researchers often assume that seawater 234U/238U has remained constant throughout the late Pleistocene. Coral specimens whose U-series ages yield an initial 234U/238U value that is significantly different than modern seawater are considered altered. Several studies have demonstrated that coral initial 234U/238U and, hence, seawater 234U/238U may have varied significantly on glacial-interglacial timescales, but the cause of this variability is subject to debate. To evaluate the pattern and mechanisms of 234U/238U variability in seawater over the last glacial cycle, we draw upon a compilation of U-series measurements of shallow and deep water corals to better define the observed variability. Observed trends from the coral record will be assessed using a simple two-box model of the ocean to determine how changes to the ocean's uranium isotope budget during glacial cycles can explain shifts in seawater 234U/238U. An improved understanding the evolution of seawater 234U/238U composition will enable more robust interpretations of both closed-system and open-system ages for corals. Such interpretations of U-series ages are essential to the development of robust chronologies for climate and sea level change and for improving the calibration of the radiocarbon timescale.

  6. A procedural manual for measurement of uranium and thorium isotopes utilizing the USGS-Stanford Finnegan Mat 262

    USGS Publications Warehouse

    Shamp, Donald D.

    2001-01-01

    Over the past several decades investigators have extensively examined the 238U-234U- 230Th systematics of a variety of geologic materials using alpha spectroscopy. Analytical uncertainty for 230Th by alpha spectroscopy has been limited to about 2% (2σ). The advantage of thermal ionization mass spectroscopy (TIMS), introduced by Edwards and co-workers in the late 1980’s is the increased detectability of these isotopes by a factor of ~200, and decreases in the uncertainty for 230Th to about 5‰ (2σ) error. This report is a procedural manual for using the USGS-Stanford Finnegan-Mat 262 TIMS to collect and isolate Uranium and Thorium isotopic ratio data. Chemical separation of Uranium and Thorium from the sample media is accomplished using acid dissolution and then processed using anion exchange resins. The Finnegan-Mat262 Thermal Ionization Mass Spectrometer (TIMS) utilizes a surface ionization technique in which nitrates of Uranium and Thorium are placed on a source filament. Upon heating, positive ion emission occurs. The ions are then accelerated and focused into a beam which passes through a curved magnetic field dispersing the ions by mass. Faraday cups and/or an ion counter capture the ions and allow for quantitative analysis of the various isotopes.

  7. Behavior of isotope (18O/16O, 234U/238U) systems during the formation of uranium deposits of the "sandstone" type

    NASA Astrophysics Data System (ADS)

    Golubev, V. N.; Dubinina, E. O.; Chernyshev, I. V.; Ikonnikova, T. A.

    2016-01-01

    The uneven character of the distribution of 18O/16O and 234U/238U values was established in the vertical cross section of the productive sequence of the Dybryn uranium deposit (Vitim uranium-ore region, Buryatia). Both a deficiency and an excess of 234U in relation to the equilibrium 234U/238U ratio in the vertical sequence may provide evidence for the extremely low rate of the infiltration water flow. The behavior of oxygen isotope characteristics for different size fractions of terrigenous rocks provides evidence for active uranium redistribution and openness of the isotope system of this element during interaction of terrigenous-sedimentary rocks with infiltration waters.

  8. Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia

    NASA Astrophysics Data System (ADS)

    Tissot, François L. H.; Dauphas, Nicolas

    2015-10-01

    The 238U/235U isotopic composition of uranium in seawater can provide important insights into the modern U budget of the oceans. Using the double spike technique and a new data reduction method, we analyzed an array of seawater samples and 41 geostandards covering a broad range of geological settings relevant to low and high temperature geochemistry. Analyses of 18 seawater samples from geographically diverse sites from the Atlantic and Pacific oceans, Mediterranean Sea, Gulf of Mexico, Persian Gulf, and English Channel, together with literature data (n = 17), yield a δ238U value for modern seawater of -0.392 ± 0.005‰ relative to CRM-112a. Measurements of the uranium isotopic compositions of river water, lake water, evaporites, modern coral, shales, and various igneous rocks (n = 64), together with compilations of literature data (n = 380), allow us to estimate the uranium isotopic compositions of the various reservoirs involved in the modern oceanic uranium budget, as well as the fractionation factors associated with U incorporation into those reservoirs. Because the incorporation of U into anoxic/euxinic sediments is accompanied by large isotopic fractionation (ΔAnoxic/Euxinic-SW = +0.6‰), the size of the anoxic/euxinic sink strongly influences the δ238U value of seawater. Keeping all other fluxes constant, the flux of uranium in the anoxic/euxinic sink is constrained to be 7.0 ± 3.1 Mmol/yr (or 14 ± 3% of the total flux out of the ocean). This translates into an areal extent of anoxia into the modern ocean of 0.21 ± 0.09% of the total seafloor. This agrees with independent estimates and rules out a recent uranium budget estimate by Henderson and Anderson (2003). Using the mass fractions and isotopic compositions of various rock types in Earth's crust, we further calculate an average δ238U isotopic composition for the continental crust of -0.29 ± 0.03‰ corresponding to a 238U/235U isotopic ratio of 137.797 ± 0.005. We discuss the implications of

  9. Organic matter and containment of uranium and fissiogenic isotopes at the Oklo natural reactors

    USGS Publications Warehouse

    Nagy, B.; Gauthier-Lafaye, F.; Holliger, P.; Davis, D.W.; Mossman, D.J.; Leventhal, J.S.; Rigali, M.J.; Parnell, J.

    1991-01-01

    SOME of the Precambrian natural fission reactors at Oklo in Gabon contain abundant organic matter1,2, part of which was liquefied at the time of criticality and subsequently converted to a graphitic solid3,4. The liquid organic matter helps to reduce U(VI) to U(IV) from aqueous solutions, resulting in the precipitation of uraninite5. It is known that in the prevailing reactor environments, precipitated uraninite grains incorporated fission products. We report here observations which show that these uraninite crystals were held immobile within the resolidified, graphitic bitumen. Unlike water-soluble (humic) organic matter, the graphitic bituminous organics at Oklo thus enhanced radionu-clide containment. Uraninite encased in solid graphitic matter in the organic-rich reactor zones lost virtually no fissiogenic lan-thanide isotopes. The first major episode of uranium and lead migration was caused by the intrusion of a swarm of adjacent dolerite dykes about 1,100 Myr after the reactors went critical. Our results from Oklo imply that the use of organic, hydrophobic solids such as graphitic bitumen as a means of immobilizing radionuclides in pretreated nuclear waste warrants further investigation. ?? 1991 Nature Publishing Group.

  10. Isotopic fractionation during leaching of impure carbonates and their effect on uranium series dating

    NASA Astrophysics Data System (ADS)

    Alcaraz Pelegrina, J. M.; Martínez-Aguirre, A.

    2005-12-01

    Experiments were designed to evaluate the behaviour of detritus during the leaching of impure carbonates by applying the U-Th isochron technique. We used one natural detritus and a pure, well-dated CaCO 3, alone and in artificial mixtures. One set of experiments was designed to study the effects of sample pre-treatment on the detritus and a second set to examine the effect of acid attacks on both the carbonate and the detritus fractions in a mixture of constant proportions. For both sets of data, the extracted fraction from the detritus was calculated for 238U, 234U, 230Th and 232Th and their constancy established. These conditions are necessary to apply the L/L method [Schwarcz, H.P., Latham, A.G., 1989. Dirty calcites. 1.-Uranium-series dating of contaminated calcite using leachates alone. Chemical Geology (Isotopes Geoscience Section) 80, 35-43] for U/Th dating. Finally, the L/L method was applied to the artificial impure carbonate and the resulting age is found in agreement with the age of the pure carbonate sample. We concluded that conditions of the L/L method to be applied for ageing impure carbonates hold.

  11. Uranium-lead isotope systematics of Mars inferred from the basaltic shergottite QUE 94201

    SciTech Connect

    Gaffney, A M; Borg, L E; Connelly, J N

    2006-12-22

    Uranium-lead ratios (commonly represented as {sup 238}U/{sup 204}Pb = {mu}) calculated for the sources of martian basalts preserve a record of petrogenetic processes that operated during early planetary differentiation and formation of martian geochemical reservoirs. To better define the range of {mu} values represented by the source regions of martian basalts, we completed U-Pb elemental and isotopic analyses on whole rock, mineral and leachate fractions from the martian meteorite Queen Alexandra Range 94201 (QUE 94201). The whole rock and silicate mineral fractions have unradiogenic Pb isotopic compositions that define a narrow range ({sup 206}Pb/{sup 204}Pb = 11.16-11.61). In contrast, the Pb isotopic compositions of weak HCl leachates are more variable and radiogenic. The intersection of the QUE 94201 data array with terrestrial Pb in {sup 206}Pb/{sup 204}Pb-{sup 207}Pb/{sup 204}Pb-{sup 208}Pb/{sup 204}Pb compositional space is consistent with varying amounts of terrestrial contamination in these fractions. We calculate that only 1-7% contamination is present in the purified silicate mineral and whole rock fractions, whereas the HCl leachates contain up to 86% terrestrial contamination. Despite the contamination, we are able to use the U-Pb data to determine the initial {sup 206}Pb/{sup 204}Pb of QUE 94201 (11.086 {+-} 0.008) and calculate the {mu} value of the QUE 94201 mantle source to be 1.823 {+-} 0.008. This is the lowest {mu} value calculated for any martian basalt source, and, when compared to the highest values determined for martian basalt sources, indicates that {mu} values in martian source reservoirs vary by at least 100%. The range of source {mu} values further indicates that the {mu} value of bulk silicate Mars is approximately three. The amount of variation in the {mu} values of the mantle sources ({mu} {approx} 2-4) is greater than can be explained by igneous processes involving silicate phases alone. We suggest the possibility that a small

  12. Isolation and Puification of Uranium Isotopes for Measurement by Mass-Spectrometry (233, 234, 235, 236, 238U) and Alpha Spectrometry (232U)

    SciTech Connect

    Marinelli, R; Hamilton, T; Brown, T; Marchetti, A; Williams, R; Tumey, S

    2006-05-30

    This report describes a standardized methodology used by researchers from the Center for Accelerator Mass Spectrometry (CAMS) (Energy and Environment Directorate) and the Environmental Radiochemistry Group (Chemistry and Materials Science Directorate) at the Lawrence Livermore National Laboratory (LLNL) for the full isotopic analysis of uranium from solution. The methodology has largely been developed for use in characterizing the uranium composition of selected nuclear materials but may also be applicable to environmental studies and assessments of public, military or occupational exposures to uranium using in-vitro bioassay monitoring techniques. Uranium isotope concentrations and isotopic ratios are measured using a combination of Multi Collector Inductively Coupled Plasma Mass Spectrometry (MC ICP-MS), Accelerator Mass Spectrometry (AMS) and Alpha Spectrometry.

  13. Groundwater Ages and Stable Isotope Fingerprints of Contaminated Water to Examine Potential Solute Sources at a Uranium Processing Mill

    NASA Astrophysics Data System (ADS)

    Hurst, T. G.; Solomon, D. K.

    2007-12-01

    To evaluate sources of high solute concentrations in groundwater near a uranium processing facility, groundwater recharge dates are correlated to specific solute concentrations and depth in the water column. Stable isotopes are also used as potential fingerprints of water sourced from mill tailing cells. Passive diffusion samplers, to be analyzed for 3He/4He ratio, were deployed in 15 different wells with samplers at two depths in the saturated interval. Low-flow purging and sampling was then conducted to isolate sampling points at different depths in the wells, with sampling at multiple depths being completed in 4 of the 15 wells sampled. Laboratory analyses were conducted for CFC recharge age, as well as T/3He recharge age. Contract laboratories analyzed for: deuterium and oxygen-18 isotopes of water; sulfur-34 and oxygen-18 isotopes of sulfate; trace metals uranium, manganese, and selenium; and nitrate and sulfate. Analysis for 235U/238U isotope ratios will be conducted to further identify fingerprint signals of source water. Groundwater recharge ages determined using CFC analysis show some vertical stratification in ages across the water column. Upon initial data processing and analysis, measured CFC ages ranged from 30 to 40 years within the water column of one well to only several years difference in another well. Additional results for trace metal concentrations, stable isotope ratios, and T/3He recharge ages will be reported when results are received. Further post-processing of CFC laboratory analysis and noble gas analyses will provide greater clarity as to groundwater ages within the aquifer and, combined with field pumping data, will allow for a comprehensive groundwater model to be constructed. This study provides great insight to potential mine tailings leakage problems and using isotopes and groundwater age dating techniques as a means of tracing contaminated groundwater to the leakage source. Utilizing stable isotopes of water and sulfate, combined

  14. NUCLEAR ISOTOPIC DILUTION OF HIGHLY ENRICHED URANIUM BY DRY BLENDING VIA THE RM-2 MILL TECHNOLOGY

    SciTech Connect

    Raj K. Rajamani; Sanjeeva Latchireddi; Vikas Devrani; Harappan Sethi; Roger Henry; Nate Chipman

    2003-08-01

    DOE has initiated numerous activities to focus on identifying material management strategies to disposition various excess fissile materials. In particular the INEEL has stored 1,700 Kg of offspec HEU at INTEC in CPP-651 vault facility. Currently, the proposed strategies for dispositioning are (a) aqueous dissolution and down blending to LEU via facilities at SRS followed by shipment of the liquid LEU to NFS for fabrication into LWR fuel for the TVA reactors and (b) dilution of the HEU to 0.9% for discard as a waste stream that would no longer have a criticality or proliferation risk without being processed through some type of enrichment system. Dispositioning this inventory as a waste stream via aqueous processing at SRS has been determined to be too costly. Thus, dry blending is the only proposed disposal process for the uranium oxide materials in the CPP-651 vault. Isotopic dilution of HEU to typically less than 20% by dry blending is the key to solving the dispositioning issue (i.e., proliferation) posed by HEU stored at INEEL. RM-2 mill is a technology developed and successfully tested for producing ultra-fine particles by dry grinding. Grinding action in RM-2 mill produces a two million-fold increase in the number of particles being blended in a centrifugal field. In a previous study, the concept of achieving complete and adequate blending and mixing (i.e., no methods were identified to easily separate and concentrate one titanium compound from the other) in remarkably short processing times was successfully tested with surrogate materials (titanium dioxide and titanium mono-oxide) with different particle sizes, hardness and densities. In the current project, the RM-2 milling technology was thoroughly tested with mixtures of natural uranium oxide (NU) and depleted uranium oxide (DU) stock to prove its performance. The effects of mill operating and design variables on the blending of NU/DU oxides were evaluated. First, NU and DU both made of the same oxide

  15. Direct isotope ratio analysis of individual uranium-plutonium mixed particles with various U/Pu ratios by thermal ionization mass spectrometry.

    PubMed

    Suzuki, Daisuke; Esaka, Fumitaka; Miyamoto, Yutaka; Magara, Masaaki

    2015-02-01

    Uranium and plutonium isotope ratios in individual uranium-plutonium (U-Pu) mixed particles with various U/Pu atomic ratios were analyzed without prior chemical separation by thermal ionization mass spectrometry (TIMS). Prior to measurement, micron-sized particles with U/Pu ratios of 1, 5, 10, 18, and 70 were produced from uranium and plutonium certified reference materials. In the TIMS analysis, the peaks of americium, plutonium, and uranium ion signals were successfully separated by continuously increasing the evaporation filament current. Consequently, the uranium and plutonium isotope ratios, except the (238)Pu/(239)Pu ratio, were successfully determined for the particles at all U/Pu ratios. This indicates that TIMS direct analysis allows for the measurement of individual U-Pu mixed particles without prior chemical separation. PMID:25479434

  16. Uranium*

    NASA Astrophysics Data System (ADS)

    Grenthe, Ingmar; Drożdżyński, Janusz; Fujino, Takeo; Buck, Edgar C.; Albrecht-Schmitt, Thomas E.; Wolf, Stephen F.

    Uranium compounds have been used as colorants since Roman times (Caley, 1948). Uranium was discovered as a chemical element in a pitchblende specimen by Martin Heinrich Klaproth, who published the results of his work in 1789. Pitchblende is an impure uranium oxide, consisting partly of the most reduced oxide uraninite (UO2) and partly of U3O8. Earlier mineralogists had considered this mineral to be a complex oxide of iron and tungsten or of iron and zinc, but Klaproth showed by dissolving it partially in strong acid that the solutions yielded precipitates that were different from those of known elements. Therefore he concluded that it contained a new element (Mellor, 1932); he named it after the planet Uranus, which had been discovered in 1781 by William Herschel, who named it after the ancient Greek deity of the Heavens.

  17. Determination of total and isotopic uranium by inductively coupled plasma-mass spectrometry at the Fernald Environmental Management Project

    SciTech Connect

    Miller, F.L.; Bolin, R.N.; Feller, M.T.; Danahy, R.J.

    1995-04-01

    At the Fernald Environmental Management Project (FEMP) in southwestern Ohio, ICP-mass spectrometry (ICP-MS), with sample introduction by peristaltic pumping, is used to determine total and isotopic uranium (U-234, U-235, U-236 and U-238) in soil samples. These analyses are conducted in support of the environmental cleanup of the FEMP site. Various aspects of the sample preparation and instrumental analysis will be discussed. Initial sample preparation consists of oven drying to determine moisture content, and grinding and rolling to homogenize the sample. This is followed by a nitric/hydrofluoric acid digestion to bring the uranium in the sample into solution. Bismuth is added to the sample prior to digestion to monitor for losses. The total uranium (U-238) content of this solution and the U{sup 235}/U{sup 238} ratio are measured on the first pass through the ICP-MS. To determine the concentration of the less abundant U{sup 234} and U{sup 236} isotopes, the digestate is further concentrated by using Eichrom TRU-Spec extraction columns before the second pass through the ICP-MS. Quality controls for both the sample preparation and instrumental protocols will also be discussed. Finally, an explanation of the calculations used to report the data in either weight percent or activity units will be given.

  18. Design Study for a Low-Enriched Uranium Core for the High Flux Isotope Reactor, Annual Report for FY 2006

    SciTech Connect

    Primm, R. T.; Ellis, R. J.; Gehin, J. C.; Clarno, K. T.; Williams, K. A.; Moses, D. L.

    2006-11-01

    Neutronics and thermal-hydraulics studies show that, for equivalent operating power [85 MW(t)], a low-enriched uranium (LEU) fuel cycle based on uranium-10 wt % molybdenum (U-10Mo) metal foil with radially, “continuously graded” fuel meat thickness results in a 15% reduction in peak thermal flux in the beryllium reflector of the High Flux Isotope Reactor (HFIR) as compared to the current highly enriched uranium (HEU) cycle. The uranium-235 content of the LEU core is almost twice the amount of the HEU core when the length of the fuel cycle is kept the same for both fuels. Because the uranium-238 content of an LEU core is a factor of 4 greater than the uranium-235 content, the LEU HFIR core would weigh 30% more than the HEU core. A minimum U-10Mo foil thickness of 84 μm is required to compensate for power peaking in the LEU core although this value could be increased significantly without much penalty. The maximum U-10Mo foil thickness is 457μm. Annual plutonium production from fueling the HFIR with LEU is predicted to be 2 kg. For dispersion fuels, the operating power for HFIR would be reduced considerably below 85 MW due to thermal considerations and due to the requirement of a 26-d fuel cycle. If an acceptable fuel can be developed, it is estimated that $140 M would be required to implement the conversion of the HFIR site at Oak Ridge National Laboratory from an HEU fuel cycle to an LEU fuel cycle. To complete the conversion by fiscal year 2014 would require that all fuel development and qualification be completed by the end of fiscal year 2009. Technological development areas that could increase the operating power of HFIR are identified as areas for study in the future.

  19. Uranium isotope dynamics across salinity and redox gradients in a coastal aquifer: implications for the oceanic uranium budget

    NASA Astrophysics Data System (ADS)

    Linhoff, B.; Charette, M. A.; Thompson, W. G.

    2014-12-01

    To balance the ocean's uranium budget it may be necessary to invoke submarine groundwater discharge as a major source for uranium. However, uranium removal from seawater has been observed in coastal aquifers where steep redox gradients at the seawater-freshwater mixing zone result in the reduction of soluble U(IV) to insoluble U(IV). We investigated uranium cycling in groundwater within a permeable sand subterranean estuary in Waquoit Bay, MA using major and trace element chemistry as well as ∂234U measurements. Groundwater and sediment samples were collected across the seawater-freshwater mixing zone. In the groundwater samples uranium does not behave conservatively. During mixing it is removed in the intermediate salinities (3-4 m; 2-12 salinity; 0.1 nM U) and enriched in higher salinities (4-6 m; 20-25 salinity; 32 nM) while in salinities >25, uranium is again removed (7-8 m; 8 nM). Geochemical modeling suggests that U is removed at the seawater-freshwater interface by adsorption to Mn-oxides (3-4 m) while in the deeper saline aquifer (7-8 m), U is removed through reduction from U(VI) to U(IV). Surprisingly, while ∂234U is above secular equilibrium in both the freshwater and seawater, within the intermediate salinities ∂234U is depleted below secular equilibrium (as much as ∂234U = -50). Sediment samples were subjected to a partial leach to extract surface-exchangeable U. This leach was analyzed for ∂234U and found to be highly depleted (∂234U -80 - -20). Based on the depleted ∂234U of the sediment leaches and groundwater, we hypothesize that the high U concentrations observed within the intermediate salinities likely have a sediment source. This also implies that U within this intermediate salinity zone must have a long residence time relative to groundwater-surface water exchange rates. This might be possible if redox boundaries and Mn-oxides act as a barrier to U in the intermediate salinities allowing U leached from sediments to accumulate

  20. Study of radioactive isotopes of beryllium, polonium, uranium, and plutonium in the atmosphere

    SciTech Connect

    Lee, S.C.

    1986-01-01

    Radiochemical measurements were carried out for /sup 239.240/Pu in a total of 94 rain and snow samples collected at Fayetteville (36/sup 0/ N, 94/sup 0/W), Arkansas, during the period between May 1983 and November 1985. The concentrations of /sup 7/Be in most of these samples were also measured and these results were compared with previous samples. Average concentrations of cosmic-ray-produced radionuclide /sup 7/Be in rain remained fairly constant year after year. The annual rate of /sup 7/Be deposition at Fayetteville, Arkansas, was calculated from these data to be 5.2 dpm/cm/sup 2//year, which corresponds to a value of 2.8 x 10/sup -2/ atoms/cm/sup 2//second for the /sup 7/Be production rate in the atmosphere. The concentrations of bomb-produced radionuclides such as /sup 89/Sr, /sup 90/Sr and /sup 239.240/Pu in rain have drastically decreased since the last nuclear test explosion was conducted by the government of People's Republic of China in 1980. The concentrations of uranium isotopes and radon daughters in rain, on the other hand, were found to be affected by atmospheric injections of volcanic ashes from the 1980 eruption of Mount St. Helens and the 1982 eruption of El Chichon volcano in Mexico. Moreover, the burnups of the nuclear-powered Soviet satellites have caused marked increases in the levels of /sup 235/U and /sup 234/U in some of the rain samples. A sharp increase in the /sup 210/Po//sup 7/Be ratio in rain samples collected toward the end of 1980 and the beginning of 1981 was attributed to an atmospheric injection of /sup 210/Po from a series of major eruptions of Mount St. Helens.

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

    SciTech Connect

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

    2012-03-01

    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.

  2. Uniform deposition of uranium hexafluoride (UF6): Standardized mass deposits and controlled isotopic ratios using a thermal fluorination method.

    PubMed

    McNamara, Bruce K; O'Hara, Matthew J; Casella, Andrew M; Carter, Jennifer C; Addleman, R Shane; MacFarlan, Paul J

    2016-07-01

    We report a convenient method for the generation of volatile uranium hexafluoride (UF6) from solid uranium oxides and other U compounds, followed by uniform deposition of low levels of UF6 onto sampling coupons. Under laminar flow conditions, UF6 is shown to interact with surfaces within a fixed reactor geometry to a highly predictable degree. We demonstrate the preparation of U deposits that range between approximately 0.01 and 500ngcm(-2). The data suggest the method can be extended to creating depositions at the sub-picogramcm(-2) level. The isotopic composition of the deposits can be customized by selection of the U source materials and we demonstrate a layering technique whereby two U solids, each with a different isotopic composition, are employed to form successive layers of UF6 on a surface. The result is an ultra-thin deposit that bears an isotopic signature that is a composite of the two U sources. The reported deposition method has direct application to the development of unique analytical standards for nuclear safeguards and forensics. Further, the method allows access to very low atomic or molecular coverages of surfaces. PMID:27154668

  3. Molecular marker and stable carbon isotope analyses of carbonaceous Ambassador uranium ores of Mulga Rock in Western Australia

    NASA Astrophysics Data System (ADS)

    Jaraula, C.; Schwark, L.; Moreau, X.; Grice, K.; Bagas, L.

    2013-12-01

    Mulga Rock is a multi-element deposit containing uranium hosted by Eocene peats and lignites deposited in inset valleys incised into Permian rocks of the Gunbarrel Basin and Precambrian rocks of the Yilgarn Craton and Albany-Fraser Orogen. Uranium readily adsorbs onto minerals or phytoclasts to form organo-uranyl complexes. This is important in pre-concentrating uranium in this relatively young ore deposit with rare uraninite [UO2] and coffinite [U(SiO4)1-x(OH)4x], more commonly amorphous and sub-micron uranium-bearing particulates. Organic geochemical and compound-specific stable carbon isotope analyses were conducted to identify possible associations of molecular markers with uranium accumulation and to recognize effect(s) of ionizing radiation on molecular markers. Samples were collected from the Ambassador deposit containing low (<200 ppm) to high (>2000 ppm) uranium concentrations. The bulk rock C/N ratios of 82 to 153, Rock-Eval pyrolysis yields of 316 to 577 mg hydrocarbon/g TOC (Hydrogen Index, HI) and 70 to 102 mg CO2/g TOC (Oxygen Index, OI) are consistent with a terrigenous and predominantly vascular plant OM source deposited in a complex shallow water system, ranging from lacustrine to deltaic, swampy wetland and even shallow lake settings as proposed by previous workers. Organic solvent extracts were separated into saturated hydrocarbon, aromatic hydrocarbon, ketone, and a combined free fatty acid and alcohol fraction. The molecular profiles appear to vary with uranium concentration. In samples with relatively low uranium concentrations, long-chain n-alkanes, alcohols and fatty acids derived from epicuticular plant waxes dominate. The n-alkane distributions (C27 to C31) reveal an odd/even preference (Carbon Preference Index, CPI=1.5) indicative of extant lipids. Average δ13C of -27 to -29 ‰ for long-chain n-alkanes is consistent with a predominant C3 plant source. Samples with relatively higher uranium concentrations contain mostly intermediate

  4. Low-Enriched Uranium Fuel Design with Two-Dimensional Grading for the High Flux Isotope Reactor

    SciTech Connect

    Ilas, Germina; Primm, Trent

    2011-05-01

    An engineering design study of the conversion of the High Flux Isotope Reactor (HFIR) from high-enriched uranium (HEU) to low-enriched uranium (LEU) fuel is ongoing at Oak Ridge National Laboratory. The computational models developed during fiscal year 2010 to search for an LEU fuel design that would meet the requirements for the conversion and the results obtained with these models are documented and discussed in this report. Estimates of relevant reactor performance parameters for the LEU fuel core are presented and compared with the corresponding data for the currently operating HEU fuel core. The results obtained indicate that the LEU fuel design would maintain the current performance of the HFIR with respect to the neutron flux to the central target region, reflector, and beam tube locations under the assumption that the operating power for the reactor fueled with LEU can be increased from the current value of 85 MW to 100 MW.

  5. NGSI FY15 Final Report. Innovative Sample Preparation for in-Field Uranium Isotopic Determinations

    SciTech Connect

    Yoshida, Thomas M.; Meyers, Lisa

    2015-11-10

    Our FY14 Final Report included an introduction to the project, background, literature search of uranium dissolution methods, assessment of commercial off the shelf (COTS) automated sample preparation systems, as well as data and results for dissolution of bulk quantities of uranium oxides, and dissolution of uranium oxides from swipe filter materials using ammonium bifluoride (ABF). Also, discussed were reaction studies of solid ABF with uranium oxide that provided a basis for determining the ABF/uranium oxide dissolution mechanism. This report details the final experiments for optimizing dissolution of U3O8 and UO2 using ABF and steps leading to development of a Standard Operating Procedure (SOP) for dissolution of uranium oxides on swipe filters.

  6. Investigating Uranium Mobility Using Stable Isotope Partitioning of 238U/235U and a Reactive Transport Model

    NASA Astrophysics Data System (ADS)

    Bizjack, M.; Johnson, T. M.; Druhan, J. L.; Shiel, A. E.

    2015-12-01

    We report a numerical reactive transport model which explicitly incorporates the effectively stable isotopes of uranium (U) and the factors that influence their partitioning in bioactive systems. The model reproduces trends observed in U isotope ratios and concentration measurements from a field experiment, thereby improving interpretations of U isotope ratios as a tracer for U reactive transport. A major factor contributing to U storage and transport is its redox state, which is commonly influenced by the availability of organic carbon to support metal-reducing microbial communities. Both laboratory and field experiments have demonstrated that biogenic reduction of U(VI) fractionates the stable isotope ratio 238U/235U, producing an isotopically heavy solid U(IV) product. It has also been shown that other common reactive transport processes involving U do not fractionate isotopes to a consistently measurable level, which suggests the capacity to quantify the extent of bioreduction occurring in groundwater containing U using 238U/235U ratios. A recent study of a U bioremediation experiment at the Rifle IFRC site (Colorado, USA) applied Rayleigh distillation models to quantify U stable isotope fractionation observed during acetate amendment. The application of these simplified models were fit to the observations only by invoking a "memory-effect," or a constant source of low-concentration, unfractionated U(VI). In order to more accurately interpret the measured U isotope ratios, we present a multi-component reactive transport model using the CrunchTope software. This approach is capable of quantifying the cycling and partitioning of individual U isotopes through a realistic network of transport and reaction pathways including reduction, oxidation, and microbial growth. The model incorporates physical heterogeneity of the aquifer sediments through zones of decreased permeability, which replicate the observed bromide tracer, major ion chemistry, U concentration, and U

  7. Determination of lead, uranium, thorium, and thallium in silicate glass standard materials by isotope dilution mass spectrometry

    USGS Publications Warehouse

    Barnes, I.L.; Garner, E.L.; Gramlich, J.W.; Moore, L.J.; Murphy, T.J.; Machlan, L.A.; Shields, W.R.; Tatsumoto, M.; Knight, R.J.

    1973-01-01

    A set of four standard glasses has been prepared which have been doped with 61 different elements at the 500-, 50-, 1-, and 0.02-ppm level. The concentrations of lead, uranium, thorium, and thallium have been determined by isotope dilution mass spectrometry at a number of points in each of the glasses. The results obtained from independent determinations in two laboratories demonstrate the homogeneity of the samples and that precision of the order of 0.5% (95% L.E.) may be obtained by the method even at the 20-ppb level for these elements. The chemical and mass spectrometric procedures necessary are presented.

  8. Method for determination of uranium isotopes in environmental samples by liquid-liquid extraction with triisooctylamine/xylene in hydrochloric media and alpha spectrometry.

    PubMed

    Popov, L

    2012-10-01

    Alternative method for determination of uranium isotopes in various environmental samples is presented. The method is based on total decomposition of the solid materials and preconcentration of liquid samples. The separation of uranium from interfering radionuclides and stable matrix elements is attained by liquid-liquid extraction with triisooctylamine/xylene in hydrochloric media. After the additional removal of stable iron by extraction with diisopropyl ether, purified uranium is electrodeposited on stainless steel disks and measured by alpha spectrometry. The analytical method has been successfully applied to the determination of uranium isotopes in water and bottom sediments from the rivers Danube, Ogosta and Tzibritza in Northwestern Bulgaria. The analytical quality was checked by analyzing reference materials with different matrices. PMID:22871440

  9. Determining the isotopic compositions of uranium and fission products in radioactive environmental microsamples using laser ablation ICP-MS with multiple ion counters.

    PubMed

    Boulyga, Sergei F; Prohaska, Thomas

    2008-01-01

    This paper presents the application of a multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS)--a Nu Plasma HR--equipped with three ion-counting multipliers and coupled to a laser ablation system (LA) for the rapid and sensitive determination of the 235U/238U, 236U/238U, 145Nd/143Nd, 146Nd/143Nd, 101Ru/(99Ru+99Tc) and 102Ru/(99Ru+99Tc) isotope ratios in microsamples collected in the vicinity of Chernobyl. Microsamples with dimensions ranging from a hundred mum to about 1 mm and with surface alpha activities of 3-38 mBq were first identified using nuclear track radiography. U, Nd and Ru isotope systems were then measured sequentially for the same microsample by LA-MC-ICP-MS. The application of a zoom ion optic for aligning the ion beams into the ion counters allows fast switching between different isotope systems, which enables all of the abovementioned isotope ratios to be measured for the same microsample within a total analysis time of 15-20 min (excluding MC-ICP-MS optimization and calibration). The 101Ru/(99Ru+99Tc) and 102Ru/(99Ru+99Tc) isotope ratios were measured for four microsamples and were found to be significantly lower than the natural ratios, indicating that the microsamples were contaminated with the corresponding fission products (Ru and Tc). A slight depletion in 146Nd of about 3-5% was observed in the contaminated samples, but the Nd isotopic ratios measured in the contaminated samples coincided with natural isotopic composition within the measurement uncertainty, as most of the Nd in the analyzed samples originates from the natural soil load of this element. The 235U/238U and 236U/238U isotope ratios were the most sensitive indicators of irradiated uranium. The present work yielded a significant variation in uranium isotope ratios in microsamples, in contrast with previously published results from the bulk analysis of contaminated samples originating from the vicinity of Chernobyl. Thus, the 235U/238U ratios measured in ten

  10. Isotopic disequilibrium of uranium: alpha-recoil damage and preferential solution effects

    SciTech Connect

    Fleischer, R.L.

    1980-02-29

    Preferential loss of uranium-234 relative to uranium-238 from rocks into solutions has long been attributed to recoiling alpha-emitting nuclei. Direct evidence has been obtained for two mechanisms, first, recoil ejection from grains, and now release by natural etching of alpha-recoil tracks. The observations have implications for radon emanation and for the storage of alpha-emitting radioactive waste.

  11. Assessment of a sequential phase extraction procedure for uranium-series isotope analysis of soils and sediments.

    PubMed

    Suresh, P O; Dosseto, A; Handley, H K; Hesse, P P

    2014-01-01

    The study of uranium-series (U-series) isotopes in soil and sediment materials has been proposed to quantify rates and timescales of soil production and sediment transport. Previous works have studied bulk soil or sediment material, which is a complex assemblage of primary and secondary minerals and organic compounds. However, the approach relies on the fractionation between U-series isotopes in primary minerals since they were liberated from the parent rock via weathering. In addition, secondary minerals and organic compounds have their own isotopic compositions such that the composition of the bulk material may not reflect that of primary minerals. Hence, there is a need for a sample preparation procedure that allows the isolation of primary minerals in soil or fluvial sediment samples. In this study, a sequential extraction procedure to separate primary minerals from soils and sediments was assessed. The procedure was applied to standard rock sample powders (TML-3 and BCR-2) to test whether it introduced any artefactual radioactive disequilibrium. A new step was introduced to remove the clay-sized fraction (<2 µm). Significant amounts (5-14%) of U and Th were removed from the rock standards during the procedure. No significant alteration in ((234)U/(238)U) and ((230)Th/(238)U) activity ratios of the rock standards occurred during the procedure. Aliquots of soil sample were subjected to the sequential extraction process to test how each step modifies the uranium-series activity ratios and mineralogy. Although no secondary minerals were detected in the unleached soil aliquots, the sequential leaching process removed up to 17% of U and Th and modified their activity ratios by up to 3%. The modification of the activity ratios poses a demand for careful means to avoid redistribution of isotopes back to the residual phase during phase extraction. PMID:24239599

  12. Identifying the sources of subsurface contamination at the Hanford site in Washington using high-precision uranium isotopic measurements

    SciTech Connect

    Christensen, John N.; Dresel, P. Evan; Conrad, Mark E.; Maher, Kate; DePaolo, Donald J.

    2004-03-30

    In the mid-1990s, a groundwater plume of uranium (U) was detected in monitoring wells in the B-BX-BY Waste Management Area (WMA) at the Hanford Site in Washington. This area has been used since the late 1940s to store high-level radioactive waste and other products of U fuel-rod processing. Using multiple collector ICP source magnetic sector mass spectrometry (MC ICPMS) high precision uranium isotopic analyses were conducted of samples of vadose zone contamination and of groundwater. The ratios {sup 236}U/{sup 238}U, {sup 234}U/{sup 238}U and {sup 238}U/{sup 235}U are used to distinguish contaminant sources. Based on the isotopic data, the source of the groundwater contamination appears to be related to a 1951 overflow event at tank BX-102 that spilled high level U waste into the vadose zone. The U isotopic variation of the groundwater plume is a result of mixing between contaminant U from this spill and natural background U. Vadose zone U contamination at tank B-110 likely predates the recorded tank leak and can be ruled out as a source of groundwater contamination, based on the U isotopic composition. The locus of vadose zone contamination is displaced from the initial locus of groundwater contamination, indicating that lateral migration in the vadose zone was at least 8 times greater than vertical migration. The time evolution of the groundwater plume suggests an average U migration rate of {approx}0.7-0.8 m/day showing slight retardation relative to a ground water flow of {approx}1 m/day.

  13. Insights into the Galápagos plume from uranium-series isotopes of recently erupted basalts

    NASA Astrophysics Data System (ADS)

    Handley, Heather K.; Turner, Simon; Berlo, Kim; Beier, Christoph; Saal, Alberto E.

    2011-09-01

    Uranium-series isotopes (238U-230Th-226Ra-210Pb), major element, trace element, and Sr-Nd isotopic data are presented for recent (<60 years old) Galápagos archipelago basalts. Volcanic rocks from all centers studied (Fernandina, Cerro Azul, Sierra Negra, and Wolf Volcano) display 230Th excesses (4%-15%) and steep rare earth element (REE) patterns indicative of residual garnet during partial melting of their mantle source. Rare earth element modeling suggests that only a few percent of garnet is involved. Correlations between (238U/232Th), radiogenic isotopes and Nb/Zr ratio suggest that the U/Th ratio of these Galápagos volcanic rocks is primarily controlled by geochemical source variations and not fractionation during partial melting. The lowest (230Th/238U) ratio is not observed at Fernandina (the supposed center of the plume) but at the more geochemically "depleted" Wolf Volcano, further to the north. Small radium excesses are observed for all samples with (226Ra/230Th) ranging from 1.107 to 1.614. The 226Ra-230Th disequilibria do not correlate with other uranium-series parent-daughter nuclide pairs or geochemical data, suggesting modification at shallow levels on timescales relevant to the half-life of 226Ra (1600 years). The combination of 226Ra and 210Pb excesses is inconsistent with interaction of magma with cumulate material unless decoupling of 210Pb (or an intermediate daughter, such as 222Rn) occurs prior to modification of Ra-Th disequilibria. An intriguing correlation of (210Pb/226Ra)0 with Nb/Zr and radiogenic isotopes requires further investigation but suggests possible control via magmatic degassing and accumulation that may somehow be related to source heterogeneities.

  14. Technical Report on the Behavior of Trace Elements, Stable Isotopes, and Radiogenic Isotopes During the Processing of Uranium Ore to Uranium Ore Concentrate

    SciTech Connect

    Marks, N. E.; Borg, L. E.; Eppich, G. R.; Gaffney, A. M.; Genneti, V. G.; Hutcheon, I. D.; Kristo, M. J.; Lindvall, R. E.; Ramon, C.; Robel, M.; Roberts, S. K.; Schorzman, K. C.; Sharp, M. A.; Singleton, M. J.; Williams, R. W.

    2015-07-09

    The goals of this SP-1 effort were to understand how isotopic and elemental signatures behave during mining, milling, and concentration and to identify analytes that might preserve geologic signatures of the protolith ores. The impurities that are preserved through the concentration process could provide useful forensic signatures and perhaps prove diagnostic of sample origin.

  15. Uranium and thorium isotopes in the rivers of the Amazonian basin: hydrology and weathering processes

    NASA Astrophysics Data System (ADS)

    Marques, Aguinaldo N., Jr.; Al-Gharib, Iyad; Bernat, Michel; Fernex, François

    2003-01-01

    hydroxylamine extracts. As expected, the 1 in the Trombetas and Negro rivers. Such ratios probably result from the binding of dissolved uranium to solid sediment.isotopes were used as tools to evaluate the chemical weathering rate of rocks in the Amazon system, which was estimated to be 2·7 cm 1000 year

  16. Uranium isotopes and dissolved organic carbon in loess permafrost: Modeling the age of ancient ice

    NASA Astrophysics Data System (ADS)

    Ewing, S. A.; Paces, J. B.; O'Donnell, J. A.; Jorgenson, M. T.; Kanevskiy, M. Z.; Aiken, G. R.; Shur, Y.; Harden, J. W.; Striegl, R.

    2015-03-01

    The residence time of ice in permafrost is an indicator of past climate history, and of the resilience and vulnerability of high-latitude ecosystems to global change. Development of geochemical indicators of ground-ice residence times in permafrost will advance understanding of the circumstances and evidence of permafrost formation, preservation, and thaw in response to climate warming and other disturbance. We used uranium isotopes to evaluate the residence time of segregated ground ice from ice-rich loess permafrost cores in central Alaska. Activity ratios of 234U vs. 238U (234U/238U) in water from thawed core sections ranged between 1.163 and 1.904 due to contact of ice and associated liquid water with mineral surfaces over time. Measured (234U/238U) values in ground ice showed an overall increase with depth in a series of five neighboring cores up to 21 m deep. This is consistent with increasing residence time of ice with depth as a result of accumulation of loess over time, as well as characteristic ice morphologies, high segregated ice content, and wedge ice, all of which support an interpretation of syngenetic permafrost formation associated with loess deposition. At the same time, stratigraphic evidence indicates some past sediment redistribution and possibly shallow thaw among cores, with local mixing of aged thaw waters. Using measures of surface area and a leaching experiment to determine U distribution, a geometric model of (234U/238U) evolution suggests mean ages of up to ∼200 ky BP in the deepest core, with estimated uncertainties of up to an order of magnitude. Evidence of secondary coatings on loess grains with elevated (234U/238U) values and U concentrations suggests that refinement of the geometric model to account for weathering processes is needed to reduce uncertainty. We suggest that in this area of deep ice-rich loess permafrost, ice bodies have been preserved from the last glacial period (10-100 ky BP), despite subsequent fluctuations in

  17. Uranium isotopes in Pleistocene permafrost: evaluating the age of ancient ice

    NASA Astrophysics Data System (ADS)

    Ewing, S. A.; Paces, J. B.; O'Donnell, J.; Kanevskiy, M. Z.; Aiken, G.; Jorgenson, T.; Shur, Y.; Striegl, R. G.

    2010-12-01

    The age of ice in permafrost is an indicator of past climate history, and of the resilience and response of high-latitude ecosytems to global change. Methods such as radiocarbon dating and tephrachronology are limited in permafrost because they provide indirect age control, and could overestimate ages when ice is intermittently absent. Development of geochemical indicators of water/ice residence time in permafrost is critical for understanding the circumstances and primary controls of permafrost formation, preservation, and thaw in response to climate change. We analyzed uranium isotopes to evaluate the age of segregated ice in ice-rich loess permafrost (yedoma) cores from central Alaska. Activity ratios of 234U vs. sup>238U (234/238U ARs) in thawed waters exceed 1.000 due to extended contact of ice with mineral surfaces over time. Ice is expected to increase in age with depth at this location based on the presence of deep loess, cryostructures associated with syngenetic permafrost aggracation, high segregated ice content, and frequent wedge ice. These features indicate that permafrost formed syngenetically as loess was deposited. Consequently, (234/238U ARs are expected to increase with depth as recoil 234U, derived from in situ decay of (238U in loess particles, accumulates in ice without being flushed over time. Values of (234/238U ARs measured for ice from a series of five neighboring cores up to 21 m deep increase with depth, consistent with downhole increases in permafrost age. Additional variability of (234/238U ARs with depth can be attributed to variations in surface area of solids determined by analysis of particle size distribution. Radiocarbon analysis of dissolved organic carbon indicates that the ages of ice are greater than ~36ky below the upper few meters, consistent with previous work on soil organic-matter profiles in this area. Using these measured parameters, a model of (234/238U AR evolution indicates minimum ages up to a minimum of ~100ky in

  18. Sediment residence times constrained by uranium-series isotopes: A critical appraisal of the comminution approach

    NASA Astrophysics Data System (ADS)

    Handley, Heather K.; Turner, Simon; Afonso, Juan C.; Dosseto, Anthony; Cohen, Tim

    2013-02-01

    Quantifying the rates of landscape evolution in response to climate change is inhibited by the difficulty of dating the formation of continental detrital sediments. We present uranium isotope data for Cooper Creek palaeochannel sediments from the Lake Eyre Basin in semi-arid South Australia in order to attempt to determine the formation ages and hence residence times of the sediments. To calculate the amount of recoil loss of 234U, a key input parameter used in the comminution approach, we use two suggested methods (weighted geometric and surface area measurement with an incorporated fractal correction) and typical assumed input parameter values found in the literature. The calculated recoil loss factors and comminution ages are highly dependent on the method of recoil loss factor determination used and the chosen assumptions. To appraise the ramifications of the assumptions inherent in the comminution age approach and determine individual and combined comminution age uncertainties associated to each variable, Monte Carlo simulations were conducted for a synthetic sediment sample. Using a reasonable associated uncertainty for each input factor and including variations in the source rock and measured (234U/238U) ratios, the total combined uncertainty on comminution age in our simulation (for both methods of recoil loss factor estimation) can amount to ±220-280 ka. The modelling shows that small changes in assumed input values translate into large effects on absolute comminution age. To improve the accuracy of the technique and provide meaningful absolute comminution ages, much tighter constraints are required on the assumptions for input factors such as the fraction of α-recoil lost 234Th and the initial (234U/238U) ratio of the source material. In order to be able to directly compare calculated comminution ages produced by different research groups, the standardisation of pre-treatment procedures, recoil loss factor estimation and assumed input parameter values

  19. Uranium isotopes and dissolved organic carbon in loess permafrost: Modeling the age of ancient ice

    USGS Publications Warehouse

    Ewing, Stephanie A.; Paces, James B.; O'Donnell, J.A.; Jorgenson, M.T.; Kanevskiy, M.Z.; Aiken, George R.; Shur, Y.; Harden, Jennifer W.; Striegl, Rob

    2015-01-01

    The residence time of ice in permafrost is an indicator of past climate history, and of the resilience and vulnerability of high-latitude ecosystems to global change. Development of geochemical indicators of ground-ice residence times in permafrost will advance understanding of the circumstances and evidence of permafrost formation, preservation, and thaw in response to climate warming and other disturbance. We used uranium isotopes to evaluate the residence time of segregated ground ice from ice-rich loess permafrost cores in central Alaska. Activity ratios of 234U vs. 238U (234U/238U) in water from thawed core sections ranged between 1.163 and 1.904 due to contact of ice and associated liquid water with mineral surfaces over time. Measured (234U/238U) values in ground ice showed an overall increase with depth in a series of five neighboring cores up to 21 m deep. This is consistent with increasing residence time of ice with depth as a result of accumulation of loess over time, as well as characteristic ice morphologies, high segregated ice content, and wedge ice, all of which support an interpretation of syngenetic permafrost formation associated with loess deposition. At the same time, stratigraphic evidence indicates some past sediment redistribution and possibly shallow thaw among cores, with local mixing of aged thaw waters. Using measures of surface area and a leaching experiment to determine U distribution, a geometric model of (234U/238U) evolution suggests mean ages of up to ∼200 ky BP in the deepest core, with estimated uncertainties of up to an order of magnitude. Evidence of secondary coatings on loess grains with elevated (234U/238U) values and U concentrations suggests that refinement of the geometric model to account for weathering processes is needed to reduce uncertainty. We suggest that in this area of deep ice-rich loess permafrost, ice bodies have been preserved from the last glacial period (10–100 ky BP), despite subsequent

  20. Uranium Isotopes in Calcium Carbonate: A Possible Proxy for Paleo-pH and Carbonate Ion Concentration?

    NASA Astrophysics Data System (ADS)

    Chen, X.; Romaniello, S. J.; Herrmann, A. D.; Wasylenki, L. E.; Anbar, A. D.

    2015-12-01

    Natural variations of 238U/235U in marine carbonates are being explored as a paleoredox proxy. However, in order for this proxy to be robust, it is important to understand how pH and alkalinity affect the fractionation of 238U/235U during coprecipitation with calcite and aragonite. Recent work suggests that the U/Ca ratio of foraminiferal calcite may vary with seawater [CO32-] concentration due to changes in U speciation[1]. Here we explore analogous isotopic consequences in inorganic laboratory co-precipitation experiments. Uranium coprecipitation experiments with calcite and aragonite were performed at pH 8.5 ± 0.1 and 7.5 ± 0.1 using a constant addition method [2]. Dissolved U in the remaining solution was periodically collected throughout the experiments. Samples were purified with UTEVA resin and 238U/235U was determined using a 233U-236U double-spike and MC-ICP-MS, attaining a precision of ± 0.10 ‰ [3]. Small but resolvable U isotope fractionation was observed in aragonite experiments at pH ~8.5, preferentially enriching heavier U isotopes in the solid phase. 238U/235U of the dissolved U in these experiments can be fit by Rayleigh fractionation curves with fractionation factors of 1.00002 - 1.00009. In contrast, no resolvable U isotope fractionation was detected in an aragonite experiment at pH ~7.5 or in calcite experiments at either pH. Equilibrium isotope fractionation among dissolved U species is the most likely mechanism driving these isotope effects. Our quantitative model of this process assumes that charged U species are preferentially incorporated into CaCO3 relative to the neutral U species Ca2UO2(CO3)3(aq), which we hypothesize to have a lighter equilibrium U isotope composition than the charged U species. According to this model, the magnitude of U isotope fractionation should scale with the fraction of the neutral U species in the solution, in agreement with our experimental results. These findings suggest that U isotope variations in

  1. Budgets and behaviors of uranium and thorium series isotopes in the Santa Monica Basin off the California Coast

    SciTech Connect

    Yu, Lei

    1991-12-16

    Samples from three time-series sediment traps deployed in the Santa Monica Basin off the California coast were analyzed to study the flux and scavenging of uranium and thorium series isotopes. Variations of uranium and thorium series isotopes fluxes in the water column were obtained by integrating these time-series deployment results. Mass and radionuclide fluxes measured from bottom sediment traps compare favorably with fluxed determined from sediment core data. This agreement suggests that the near-bottom sediment traps are capable of collecting settling particles representative of the surface sediment. The phase distributions of {sup 234}Th in the water column were calculated by an inverse method using sediment trap data, which help to study the variations of {sup 234}Th scavenging in the water column. Scavenging and radioactive decay of {sup 234}Th are the two principal processes for balancing {sup 234}Th budget in the water column. The residence times of dissolved and particulate {sup 234}Th were determined by a {sup 234}Th scavenging model.

  2. The Role of COMSOL Toward a Low-Enriched Uranium Fuel Design for the High Flux Isotope Reactor

    SciTech Connect

    Freels, James D; Arimilli, Rao V; Lowe, Kirk T; Bodey, Isaac T

    2009-01-01

    Design and safety analyses are underway to convert the High Flux Isotope Reactor (HFIR) at the Oak Ridge National Laboratory (ORNL) from a high-enriched uranium (HEU) fuel to a low-enriched uranium (LEU) fuel. The primary constraint for the project is that the overall fuel plate dimensions and the current neutron flux performance must remain unchanged. This allows minimal impact on the facility and cost for the conversion, and provides transparency to the HFIR customer base and research projects that depend on the facility for isotopes and neutron flux. As a consequence, the LEU design demands more accuracy and less margin in the analysis efforts than the original design. Several technical disciplines are required to complete this conversion including nuclear reactor physics, heat transfer, fluid dynamics, structural mechanics, fuel fabrication, and engineering design. The role of COMSOL is to provide the fully-coupled 3D multi-physics analysis for heat transfer, turbulent flow, and structural mechanics of the fuel plates and flow channels. A goal is for COMSOL to simulate the entire fuel element array of fuel plates (171 inner, 369 outer). This paper describes the progress that has been made toward development of benchmark validation models of the existing HEU inner-element fuel plates.

  3. A combined chemical, isotopic and microstructural study of pyrite from roll-front uranium deposits, Lake Eyre Basin, South Australia

    NASA Astrophysics Data System (ADS)

    Ingham, Edwina S.; Cook, Nigel J.; Cliff, John; Ciobanu, Cristiana L.; Huddleston, Adam

    2014-01-01

    The common sulfide mineral pyrite is abundant throughout sedimentary uranium systems at Pepegoona, Pepegoona West and Pannikan, Lake Eyre Basin, South Australia. Combined chemical, isotopic and microstructural analysis of pyrite indicates variation in fluid composition, sulfur source and precipitation conditions during a protracted mineralization event. The results show the significant role played by pyrite as a metal scavenger and monitor of fluid changes in low-temperature hydrothermal systems. In-situ micrometer-scale sulfur isotope analyses of pyrite demonstrated broad-scale isotopic heterogeneity (δ34S = -43.9 to +32.4‰VCDT), indicative of complex, multi-faceted pyrite evolution, and sulfur derived from more than a single source. Preserved textures support this assertion and indicate a genetic model involving more than one phase of pyrite formation. Authigenic pyrite underwent prolonged evolution and recrystallization, evidenced by a genetic relationship between archetypal framboidal aggregates and pyrite euhedra. Secondary hydrothermal pyrite commonly displays hyper-enrichment of several trace elements (Mn, Co, Ni, As, Se, Mo, Sb, W and Tl) in ore-bearing horizons. Hydrothermal fluids of magmatic and meteoric origins supplied metals to the system but the geochemical signature of pyrite suggests a dominantly granitic source and also the influence of mafic rock types. Irregular variation in δ34S, coupled with oscillatory trace element zonation in secondary pyrite, is interpreted in terms of continuous variations in fluid composition and cycles of diagenetic recrystallization. A late-stage oxidizing fluid may have mobilized selenium from pre-existing pyrite. Subsequent restoration of reduced conditions within the aquifer caused ongoing pyrite re-crystallization and precipitation of selenium as native selenium. These results provide the first qualitative constraints on the formation mechanisms of the uranium deposits at Beverley North. Insights into

  4. Establishing a Cost Basis for Converting the High Flux Isotope Reactor from High Enriched to Low Enriched Uranium Fuel

    SciTech Connect

    Primm, Trent; Guida, Tracey

    2010-02-01

    Under the auspices of the Global Threat Reduction Initiative Reduced Enrichment for Research and Test Reactors Program, the National Nuclear Security Administration /Department of Energy (NNSA/DOE) has, as a goal, to convert research reactors worldwide from weapons grade to non-weapons grade uranium. The High Flux Isotope Reactor (HFIR) at Oak Ridge National Lab (ORNL) is one of the candidates for conversion of fuel from high enriched uranium (HEU) to low enriched uranium (LEU). A well documented business model, including tasks, costs, and schedules was developed to plan the conversion of HFIR. Using Microsoft Project, a detailed outline of the conversion program was established and consists of LEU fuel design activities, a fresh fuel shipping cask, improvements to the HFIR reactor building, and spent fuel operations. Current-value costs total $76 million dollars, include over 100 subtasks, and will take over 10 years to complete. The model and schedule follows the path of the fuel from receipt from fuel fabricator to delivery to spent fuel storage and illustrates the duration, start, and completion dates of each subtask to be completed. Assumptions that form the basis of the cost estimate have significant impact on cost and schedule.

  5. Determination of plutonium-239, thorium-232, and natural uranium isotopic concentrations in biological samples using photofission track analysis

    NASA Astrophysics Data System (ADS)

    Parry, James Roswell

    Fission track analysis (FTA) has many uses in the scientific community including but not limited to geological dating, neutron flux mapping, and dose reconstruction. The common method of fission for FTA is through neutrons from a nuclear reactor. This dissertation investigates the use of bremsstrahlung radiation produced from an electron linear accelerator to induce fission in FTA samples. This provides a means of simultaneously measuring the amount of Pu-239, U-nat, and Th-232 in a single sample. The benefit of measuring the three isotopes simultaneously is the possible elimination of costly and time consuming chemical processing for dose reconstruction samples. Samples containing the three isotopes were irradiated in two different bremsstrahlung spectra and a neutron spectrum to determine the amount of Pu-239, U-nat, and Th-232 in the samples. The reaction rate from the calibration samples and the counted fission tracks on the samples were used in determining the concentration of each isotope in the samples. The results were accurate to within a factor of two or three, showing that the method can work to predict the concentrations of multiple isotopes in a sample. The limitations of current accelerators and detectors limits the application of this specific procedure to higher concentrations of isotopes. The method detection limits for Pu-239, U-nat, and Th-232 are 20 pCi, 1 fCi, and 0.4 flCI respectively. Analysis of extremely low concentrations of isotopes would require the use of different detectors such as quartz due to the embrittlement encountered in the Lexan at high exposures. Cracking of the Texan detectors started to appear at a fluence of about 2 x 1018 electrons from the accelerator. This may be partly due to the beam stop not being an adequate thickness. The procedure is likely limited to specialty applications for the near term. However, with the world concerns of exposure to depleted uranium, this procedure may find applications in this area since

  6. Isotopic disequilibrium of uranium: alpha-recoil damage and preferential solution effects.

    PubMed

    Fleischer, R L

    1980-02-29

    Preferential loss of uranium-234 relative to uranium-238 from rocks into solutions has long been attributed to recoiling alpha-emitting nuclei. Direct evidence has been obtained for two mechanisms, first, recoil ejection from grains, and now release by natural etching of alpha-recoil tracks. The observations have implications for radon emanation and for the storage of alpha-emitting radioactive waste. PMID:17830457

  7. Chemical and isotopic studies of granitic Archean rocks, Owl Creek Mountains, Wyoming: Uranium-thorium-lead systematics of an Archean granite from the Owl Creek Mountains, Wyoming

    SciTech Connect

    Stuckless, J.S.; Nkomo, I.T.; Butt, K.A.

    1986-01-01

    Isotopic analyses of apparently unaltered whole-rock samples of a granite from the Owl Creek Mountains, Wyo., yield a lead-lead isochron age of 2730 {plus minus} 35 Ma, which is somewhat older than the age obtained by the rubidium-strontium whole-rock method. Thorium-lead data for the same samples deviate markedly from an isochronal relation; however, calculated initial {sup 208}Pb/{sup 204}Pb ratios correlate with whole-rock {delta}{sup 18}O values and lead to the conclusion that the {sup 232}Th-{sup 208}Pb data are not colinear because of an originally heterogeneous granitic magma. Relationships in the {sup 207}Pb/{sup 235}U-{sup 206}Pb/{sup 238}U system show that uranium was mobilized during early Laramide time or shortly before, such that most surface and shallow drill-core samples lost 60-80 percent of their uranium, and some fractured, deeper drill-core samples gained from 50 to 10,000 percent uranium. Fission-track maps show that much uranium is located along edges and cleavages of biotite and magnetic where it is readily accessible to oxidizing ground water. Furthermore, qualitative comparisons of uranium distribution in samples with excess radiogenic lead and in samples with approximately equilibrium amounts of uranium and lead suggest that the latter contain more uranium in these readily accessible sites. Unlike other granites that have uranium distributions and isotopic systematics similar to those observed in this study, the granite of the Owl Creek Mountains is not associated with economic uranium deposits.

  8. Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the 233U isotope in the VVER reactors using thorium and heavy water

    NASA Astrophysics Data System (ADS)

    Marshalkin, V. E.; Povyshev, V. M.

    2015-12-01

    A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium-uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D2O, H2O) is proposed. The method is characterized by efficient breeding of the 233U isotope and safe reactor operation and is comparatively simple to implement.

  9. Elemental and Isotopic Analysis of Uranium Oxide an NIST Glass Standards by FEMTOSECOND-LA-ICP-MIC-MS

    SciTech Connect

    Ebert, Chris; Zamzow, Daniel S.; McBay, Eddie H.; Bostick, Debra A.; Bajic, Stanley J.; Baldwin, David P.; Houk, R.S.

    2009-06-01

    The objective of this work was to test and demonstrate the analytical figures of merit of a femtosecond-laser ablation (fs-LA) system coupled with an inductively coupled plasma-multi-ion collector-mass spectrometer (ICP-MIC-MS). The mobile fs-LA sampling system was designed and assembled at Ames Laboratory and shipped to Oak Ridge National Laboratory (ORNL), where it was integrated with an ICP-MIC-MS. The test period of the integrated systems was February 2-6, 2009. Spatially-resolved analysis of particulate samples is accomplished by 100-shot laser ablation using a fs-pulsewidth laser and monitoring selected isotopes in the resulting ICP-MS transient signal. The capability of performing high sensitivity, spatially resolved, isotopic analyses with high accuracy and precision and with virtually no sample preparation makes fs-LA-ICP-MIC-MS valuable for the measurement of actinide isotopes at low concentrations in very small samples for nonproliferation purposes. Femtosecond-LA has been shown to generate particles from the sample that are more representative of the bulk composition, thereby minimizing weaknesses encountered in previous work using nanosecond-LA (ns-LA). The improvement of fs- over ns-LA sampling arises from the different mechanisms for transfer of energy into the sample in these two laser pulse-length regimes. The shorter duration fs-LA pulses induce less heating and cause less damage to the sample than the longer ns pulses. This results in better stoichiometric sampling (i.e., a closer correlation between the composition of the ablated particles and that of the original solid sample), which improves accuracy for both intra- and inter-elemental analysis. The primary samples analyzed in this work are (a) solid uranium oxide powdered samples having different {sup 235}U to {sup 238}U concentration ratios, and (b) glass reference materials (NIST 610, 612, 614, and 616). Solid uranium oxide samples containing {sup 235}U in depleted, natural, and enriched

  10. Desert varnish: potential for age dating via uranium-series isotopes

    SciTech Connect

    Knauss, K.G.; Ku, T.L.

    1980-01-01

    Trace metals and natural radioisotopes are measured in an unusually thick and presumed ancient desert varnish from the Colorado Plateau in Utah. Uranium and thorium concentrations in the sequence: varnish-altered rind-heartrock (Shinarump formation sandstone) indicate that uranium with little accompanying thorium is derived from external sources. The varnish forms a closed system for /sup 230/Th and /sup 231/Pa with equilibrium values for both /sup 230/Th//sup 234/U and /sup 231/Pa//sup 235/U. Selective leaching of the ferromanganese oxides followed by analysis of both the leachate and silicate residue is proposed to allow age determinations.

  11. Desert varnish: potential for age dating via uranium-series isotopes

    SciTech Connect

    Knauss, K.G.; Ku, T.L.

    1980-01-01

    Trace metals and natural radioisotopes are measured in an unusually thick and presumed ancient desert varnish from the Colorado Plateau in Utah. Uranium and thorium concentrations in the sequence: varnish--altered rind--heartrock (Shinarump formation sandstone) indicate that uranium with little accompanying thorium is derived from external sources. The varnish forms a closed system for /sup 230/Th and /sup 231/Pa with equilibrium values for both /sup 230/Th//sup 234/U and /sup 231/Pa//sup 235/U. Selective leaching of the ferromanganese oxides followed by analysis of both the leachate and silicate residue is proposed to allow age determinations.

  12. Application of copper vapour lasers for controlling activity of uranium isotopes

    NASA Astrophysics Data System (ADS)

    Barmina, E. V.; Sukhov, I. A.; Lepekhin, N. M.; Priseko, Yu S.; Filippov, V. G.; Simakin, Aleksandr V.; Shafeev, Georgii A.

    2013-06-01

    Beryllium nanoparticles are generated upon ablation of a beryllium target in water by a copper vapour laser. The average size of single crystalline nanoparticles is 12 nm. Ablation of a beryllium target in aqueous solutions of uranyl chloride leads to a significant (up to 50 %) decrease in the gamma activity of radionuclides of the uranium-238 and uranium-235 series. Data on the recovery of the gamma activity of these nuclides to new steady-state values after laser irradiation are obtained. The possibility of application of copper vapour lasers for radioactive waste deactivation is discussed.

  13. Application of copper vapour lasers for controlling activity of uranium isotopes

    SciTech Connect

    Barmina, E V; Sukhov, I A; Lepekhin, N M; Priseko, Yu S; Filippov, V G; Simakin, Aleksandr V; Shafeev, Georgii A

    2013-06-30

    Beryllium nanoparticles are generated upon ablation of a beryllium target in water by a copper vapour laser. The average size of single crystalline nanoparticles is 12 nm. Ablation of a beryllium target in aqueous solutions of uranyl chloride leads to a significant (up to 50 %) decrease in the gamma activity of radionuclides of the uranium-238 and uranium-235 series. Data on the recovery of the gamma activity of these nuclides to new steady-state values after laser irradiation are obtained. The possibility of application of copper vapour lasers for radioactive waste deactivation is discussed. (laser applications and other topics in quantum electronics)

  14. Uranium isotope systematics of ferromanganese crusts in the Pacific Ocean: Implications for the marine 238U/235U isotope system

    NASA Astrophysics Data System (ADS)

    Goto, Kosuke T.; Anbar, Ariel D.; Gordon, Gwyneth W.; Romaniello, Stephen J.; Shimoda, Gen; Takaya, Yutaro; Tokumaru, Ayaka; Nozaki, Tatsuo; Suzuki, Katsuhiko; Machida, Shiki; Hanyu, Takeshi; Usui, Akira

    2014-12-01

    Variations of 238U/235U ratio (δ238U) in sedimentary rocks have been proposed as a possible proxy for the paleo-oceanic redox conditions, although the marine δ238U system is not fully understood. Here we investigate the spatial variation of δ238U in modern ferromanganese (Fe-Mn) crusts by analyzing U isotopes in the surface (0-3 mm depth) layer of 19 Fe-Mn crusts collected from 6 seamounts in the Pacific Ocean. δ238U values in the surface layers show little variation and range from -0.59‰ to -0.69‰. The uniformity of δ238U values is consistent with the long residence time of U in modern seawater, although the δ238U values are lighter than that of present-day seawater by ∼0.24‰. The light δ238U values are consistent with the isotope offset observed in previously reported adsorption experiment of U to Mn oxide. These results indicate that removal of U from seawater to Mn oxide is responsible for the second largest U isotope fractionation in the modern marine system, and could contribute to isotopically heavy U to seawater. Depth profiles of U isotopes (δ234U and δ238U) in two Fe-Mn crusts (MR12-03_D06-R01 and MC10_CB07_B), dated by Os isotope stratigraphy, were investigated to reconstruct the evolution of the oceanic redox state during the Cenozoic. The δ238U depth profiles show very limited ranges (-0.57‰ to -0.67‰ for MR12-03_D06-R01 and -0.56‰ to -0.69‰ for MC10_CB07_B), and have values that are similar to those of the surface layers of Fe-Mn crusts. The absence of any resolvable variation in the δ238U depth profiles may suggest that the relative amounts of oxic and reducing U sinks have not varied significantly over the past 45 Myr. However, the δ234U depth profiles of the same samples show evidence for the possible redistribution of 234U after deposition. Therefore, the depth profile of δ238U in Fe-Mn crusts may have been also overprinted by later chemical exchange with pore-water or seawater, and may not reflect the paleo

  15. Demonstration of femtosecond laser ablation inductively coupled plasma mass spectrometry for uranium isotopic measurements in U-10Mo nuclear fuel foils

    SciTech Connect

    Havrilla, George Joseph; Gonzalez, Jhanis

    2015-06-10

    The use of femtosecond laser ablation inductively coupled plasma mass spectrometry was used to demonstrate the feasibility of measuring the isotopic ratio of uranium directly in U-10Mo fuel foils. The measurements were done on both the flat surface and cross sections of bare and Zr clad U-10Mo fuel foil samples. The results for the depleted uranium content measurements were less than 10% of the accepted U235/238 ratio of 0.0020. Sampling was demonstrated for line scans and elemental mapping over large areas. In addition to the U isotopic ratio measurement, the Zr thickness could be measured as well as trace elemental composition if required. A number of interesting features were observed during the feasibility measurements which could provide the basis for further investigation using this methodology. The results demonstrate the feasibility of using fs-LA-ICP-MS for measuring the U isotopic ratio in U-10Mo fuel foils.

  16. Innovative lasers for uranium isotope separation. Progress report for the period September 1, 1989--May 31, 1990

    SciTech Connect

    Brake, M.L.; Gilgenbach, R.M.

    1990-06-01

    Copper vapor lasers have important applications to uranium atomic vapor laser isotope separation (AVLIS). The authors have spent the first year of the project investigating two innovative methods of exciting/pumping copper vapor lasers which have the potential to improve the efficiency and scaling of large laser systems used in uranium isotope separation. Experimental research has focused on the laser discharge kinetics of (1) microwave and (2) electron beam excitation/pumping of large-volume copper vapor lasers. During the first year, the experiments have been designed and constructed and initial data has been taken. Highlights of some of the first year results as well as plans for the future include the following: Microwave resonant cavity produced copper vapor plasmas at 2.45 GHz, both pulsed (5 kW, 5kHz) and CW (0--500 Watts) have been investigated using heated copper chloride as the copper source. The visible emitted light has been observed and intense lines at 510.6 nm and 578.2 nm have been observed. Initial measurements of the electric field strengths have been taken with probes, the plasma volume has been measured with optical techniques, and the power has been measured with power meters. A self-consistent electromagnetic model of the cavity/plasma system which uses the above data as input shows that the copper plasma has skin depths around 100 cm, densities around 10{sup 12} {number_sign}/cc, collisional frequencies around 10{sup 11}/sec., conductivities around 0.15 (Ohm-meter){sup {minus}1}. A simple model of the heat transfer predicts temperatures of {approximately}900 K. All of these parameters indicate that microwave discharges may be well suited as a pump source for copper lasers. These preliminary studies will be continued during the second year with additional diagnostics added to the system to verify the model results. Chemical kinetics of the system will also be added to the model.

  17. The Rosetta Stone of isotope science and the uranium/lead system.

    PubMed

    De Laeter, John

    2011-01-01

    The nucleosynthetic characteristics of U and Pb, together with the interconnectivity between these elements by two radioactive decay chains, are the foundation on which the U/Pb system was able to make a unique contribution to isotope science. The Rosetta Stone is an ancient Egyptian tablet that enabled previously indecipherable hieroglyphics to be translated. In a similar manner, the isotopic investigation of the U/Pb system, by a variety of mass spectrometric instrumentation, has led to our knowledge of the age of the Earth and contributed to thermochronology. In a similar manner, climate change information has been garnered by utilizing the U-Disequilibrium Series to measure the ages of marine archives. The impact of Pb in the environment has been demonstrated in human health, particularly at the peak of leaded petrol consumption in motor vehicles in the 1970s. Variations in the isotopic composition of lead in samples enable the source of the lead to be "fingerprinted" so as to trace the history of the Pb in ice cores and aerosols. The discovery of nuclear fission of (235)U led to the development of nuclear reactors and the isotopic investigation of the Oklo natural reactors. The mass spectrometer is the modern Rosetta Stone of isotope science, which has enabled the isotopic hieroglyphics of the U/Pb system to be investigated to reveal new horizons in our understanding of nature, and to address a number of societal and environmental problems. PMID:24737630

  18. Uranium Isotope Fractionation during Oxidation of Dissolved U(iv) and Synthetic Solid UO2

    NASA Astrophysics Data System (ADS)

    Wang, X.; Johnson, T. M.; Lundstrom, C. C.

    2013-12-01

    U isotopes (238U/235U) show promise as a tool for environmental monitoring of U contamination as well as a proxy for paleo-redox conditions. However, the isotopic fractionation mechanisms of U are still poorly understood. In groundwater systems, U(VI), a mobile contaminant, can be reduced to immobile U(IV) and thus remediated. Previous work shows that 238U/235U of the remaining U(VI) changes with the extent of reduction. Therefore, U(VI) isotope composition in groundwater can potentially be used to detect and perhaps quantify the extent of reduction. However, knowing if isotopic fractionation occurs during U(IV) oxidation is equally important. First, the reduced U(IV) (either solid or as dissolved organic complexes) potentially can be reoxidized to U(VI). If isotope fractionation occurs during oxidation, it would complicate the use of U isotope composition as a monitoring technique. Further, in natural weathering processes, U(IV) minerals are oxidized to form dissolved U(VI), which is carried to rivers and eventually to the ocean and deposited in marine sediments. The weathering cycle is thus sensitive to redox conditions, meaning the sedimentary U isotope record may serve as a paleoredox indicator, provided U isotope fractionation during oxidation and reduction are well known. We conducted experiments oxidizing 2 different U(IV) species by O2 and measuring isotopic fractionation factors. In one experiment, dissolved U(IV) in 0.1 N HCl (pH 1) was oxidized by entrained air. As oxidation proceeds at pH 1, the remaining dissolved U(IV) becomes progressively enriched in 238U in a linear trend, while the product U(VI) paralleled, but was offset to 1.0‰ lighter in 238U/235U. This linear progression of both remaining reactant and product suggests equilibrium fractionation during oxidation of dissolved U(IV) by O2. A second experiment oxidized synthetic, solid UO2 (in 20 mM NaHCO3, pH 7) with entrained air. The oxidative fractionation is very weak in this case with

  19. The applicability of MGA method for depleted and natural uranium isotopic analysis in the presence of actinides (232Th, 237Np, 233Pa and 241Am).

    PubMed

    Yücel, Haluk

    2007-11-01

    The multi-group analysis (MGA) method for the determination of uranium isotopic abundances in depleted uranium (DU) and natural uranium (NU) samples is applied in this study. A set of non-destructive gamma-ray measurements of DU and NU samples were performed using a planar Ge detector. The relative abundances of 235U and 238U isotopes were compared with the declared values of the standards. The relative abundance for 235U obtained by MGA for a "clean" DU or NU sample with a content of uranium>1wt% is determined with an accuracy of about +/-5%. However, when several actinides such as 232Th, 237Np, 233Pa and 241Am are present along with uranium isotopes simulating "dirty" DU or NU, it has been observed that MGA method gives erroneous results. The 235U abundance results for the samples were 6-25 times higher than the declared values in the presence of above-mentioned actinides, since MGA is utilized the X-ray and gamma-ray peaks in the 80-130 keV energy region, covering XKalpha and XKbeta regions. After the least-squares fitting of the spectra, it is found that the increases in the intensities of the X-ray and gamma-ray peaks of uranium are remarkably larger in the complex 80-130 keV region. On the other hand, it is observed that the interferences of the actinide peaks are relatively less dominant in the higher gamma-ray region of 130-300 keV. The results imply the need for dirty DU and NU samples that the MGA method should utilize the higher energy gamma-rays (up to 1001 keV of (234m)Pa) combined with lower energies of the spectra, which may be collected in a two detector mode (a planar Ge and a high efficient coaxial Ge). PMID:17606378

  20. Direct uranium isotope ratio analysis of single micrometer-sized glass particles

    PubMed Central

    Kappel, Stefanie; Boulyga, Sergei F.; Prohaska, Thomas

    2012-01-01

    We present the application of nanosecond laser ablation (LA) coupled to a ‘Nu Plasma HR’ multi collector inductively coupled plasma mass spectrometer (MC-ICP-MS) for the direct analysis of U isotope ratios in single, 10–20 μm-sized, U-doped glass particles. Method development included studies with respect to (1) external correction of the measured U isotope ratios in glass particles, (2) the applied laser ablation carrier gas (i.e. Ar versus He) and (3) the accurate determination of lower abundant 236U/238U isotope ratios (i.e. 10−5). In addition, a data processing procedure was developed for evaluation of transient signals, which is of potential use for routine application of the developed method. We demonstrate that the developed method is reliable and well suited for determining U isotope ratios of individual particles. Analyses of twenty-eight S1 glass particles, measured under optimized conditions, yielded average biases of less than 0.6% from the certified values for 234U/238U and 235U/238U ratios. Experimental results obtained for 236U/238U isotope ratios deviated by less than −2.5% from the certified values. Expanded relative total combined standard uncertainties Uc (k = 2) of 2.6%, 1.4% and 5.8% were calculated for 234U/238U, 235U/238U and 236U/238U, respectively. PMID:22595724

  1. Design Study for a Low-enriched Uranium Core for the High Flux Isotope Reactor, Annual Report for FY 2007

    SciTech Connect

    Primm, Trent; Ellis, Ronald James; Gehin, Jess C; Ilas, Germina; Miller, James Henry; Sease, John D

    2007-11-01

    This report documents progress made during fiscal year 2007 in studies of converting the High Flux Isotope Reactor (HFIR) from highly enriched uranium (HEU) fuel to low enriched uranium fuel (LEU). Conversion from HEU to LEU will require a change in fuel form from uranium oxide to a uranium-molybdenum alloy. A high volume fraction U/Mo-in-Al fuel could attain the same neutron flux performance as with the current, HEU fuel but materials considerations appear to preclude production and irradiation of such a fuel. A diffusion barrier would be required if Al is to be retained as the interstitial medium and the additional volume required for this barrier would degrade performance. Attaining the high volume fraction (55 wt. %) of U/Mo assumed in the computational study while maintaining the current fuel plate acceptance level at the fuel manufacturer is unlikely, i.e. no increase in the percentage of plates rejected for non-compliance with the fuel specification. Substitution of a zirconium alloy for Al would significantly increase the weight of the fuel element, the cost of the fuel element, and introduce an as-yet untried manufacturing process. A monolithic U-10Mo foil is the choice of LEU fuel for HFIR. Preliminary calculations indicate that with a modest increase in reactor power, the flux performance of the reactor can be maintained at the current level. A linearly-graded, radial fuel thickness profile is preferred to the arched profile currently used in HEU fuel because the LEU fuel media is a metal alloy foil rather than a powder. Developments in analysis capability and nuclear data processing techniques are underway with the goal of verifying the preliminary calculations of LEU flux performance. A conceptual study of the operational cost of an LEU fuel fabrication facility yielded the conclusion that the annual fuel cost to the HFIR would increase significantly from the current, HEU fuel cycle. Though manufacturing can be accomplished with existing technology

  2. Validation of isotope signatures in sediments affected by anthropogenic inputs from uranium series radionuclides.

    PubMed

    San Miguel, E G; Pérez-Moreno, J P; Bolívar, J P; García-Tenorio, R

    2003-01-01

    This paper aims to show the usefulness of 226Ra/228Ra activity ratios and confirm the possibility of using 230Th/232Th activity ratios as chronological markers in sediment cores from an estuarine system strongly contaminated by discharges from non-nuclear industries (fertiliser plants). The validation was carried out using an independent, well-established dating technique based on the analysis of the 137Cs fallout profile, which comprises the same time interval as that covered by both isotope ratios. The advantage of using the 226Ra/228Ra activity ratio profile instead of the Th-isotope profile is that determination can be accomplished with a non-destructive, simpler and less time-consuming technique, because both Ra isotopes can be determined by gamma-ray spectrometry. PMID:12663212

  3. Very long hillslope transport timescales determined from uranium-series isotopes in river sediments from a large, tectonically stable catchment

    NASA Astrophysics Data System (ADS)

    Suresh, P. O.; Dosseto, A.; Hesse, P. P.; Handley, H. K.

    2014-10-01

    The uranium-series isotopic compositions of soils and sediments evolve in response to time and weathering conditions. Therefore, these isotopes can be used to constrain the timescales of river sediment transport. Catchment evolution depends on the sediment dynamic timescales, on which erosion imparts a major control. Erosion rates in tectonically stable catchments are expected to be lower than those in tectonically active catchments, implying longer sediment residence times in tectonically stable catchments. Mineralogical, elemental and isotopic data are presented for modern channel sediments, alluvial and colluvial deposits from the Murrumbidgee River, a large catchment in the passive margin highlands of south-eastern Australia and three of its tributaries from the headwaters to the alluvial plain. Low variability in Si-based Weathering Index indicates that there is little chemical weathering occurring in the Murrumbidgee River during sediment transport. However, quartz content increases and plagioclase content decreases downstream, indicating progressive mineralogical sorting and/or physical comminution with increasing transport distance. U-series isotopic ratios in the Murrumbidgee River trunk stream sediments show no systematic downstream variation. The weathering ages of sediments within the catchment were determined using a loss-gain model of U-series isotopes. Modern sediments from a headwater tributary, the Bredbo River at Frogs Hollow, have a weathering age of 76 ± 30 kyr but all other modern channel sediments from the length of the Murrumbidgee River and its main tributaries have weathering ages ∼400 ± 180 kyr. The two headwater colluvial deposits have weathering ages of 57 ± 13 and 47 ± 11 kyr, respectively. All the alluvial deposits have weathering ages similar to those of modern sediments. No downstream trend in weathering age is observed. Together with the soil residence time of up to 30 kyr for ridge-top soils at Frogs Hollow in the upper

  4. Soil formation rates determined from Uranium-series isotope disequilibria in soil profiles from the southeastern Australian highlands

    NASA Astrophysics Data System (ADS)

    Suresh, P. O.; Dosseto, A.; Hesse, P. P.; Handley, H. K.

    2013-10-01

    The sustainability of soil resources is determined by the balance between the rates of production and removal of soils. Samples from four weathering profiles at Frogs Hollow in the upper catchment area of the Murrumbidgee River (southeastern Australia) were analyzed for their uranium-series (U-series) isotopic composition to estimate soil production rates. Sequential leaching was conducted on sample aliquots to assess how U-series nuclides are distributed between primary and secondary minerals. Soil is increasingly weathered from bottom to top which is evident from the decrease in (234U/238U) ratios and increase in relative quartz content with decreasing soil depth. One soil profile shows little variation in mineralogy and U-series geochemistry with depth, explained by the occurrence of already extensively weathered saprolite, so that further weathering has minimal effect on mineralogy and geochemistry. Al2O3 is mobilized from these soils, and hence a silicon-based weathering index treating Al2O3 as mobile is introduced, which increases with decreasing soil depth, in all profiles. Leached and unleached aliquots show similar mineralogy with slight variation in relative concentrations, whereas the elemental and isotopic composition of uranium and thorium show notable differences between leached and unleached samples. Unleached samples show systematic variations in uranium-series isotopic compositions with depth compared to leached samples. This is most likely explained by the mobilization of U and Th from the samples during leaching. Soil residence times are calculated by modeling U-series activity ratios for each profile separately. Inferred timescales vary up to 30 kyr for unleached aliquots from profile F1 to up to 12 kyr for both leached and unleached aliquots from profile F2. Muscovite content shows a linear relationship with U-series derived soil residence times. This relationship provides an alternative method to estimate residence timescales for profiles with

  5. Urinary isotopic analysis in the UK Armed Forces: no evidence of depleted uranium absorption in combat and other personnel in Iraq

    PubMed Central

    Bland, D; Rona, R; Coggon, D; Anderson, J; Greenberg, N; Hull, L; Wessely, S

    2007-01-01

    Objectives To assess the distribution and risk factors of depleted uranium uptake in military personnel who had taken part in the invasion of Iraq in 2003. Methods Sector field inductively coupled plasma-mass spectrometry (SF-ICP-MS) was used to determine the uranium concentration and 238U/235U isotopic ratio in spot urine samples. The authors collected urine samples from four groups identified a priori as having different potential for exposure to depleted uranium. These groups were: combat personnel (n = 199); non-combat personnel (n = 96); medical personnel (n = 22); and “clean-up” personnel (n = 24) who had been involved in the maintenance, repair or clearance of potentially contaminated vehicles in Iraq. A short questionnaire was used to ascertain individual experience of circumstances in which depleted uranium exposure might have occurred. Results There was no statistically significant difference in the 238U/235U ratio between groups. Mean ratios by group varied from 138.0 (95% CI 137.3 to 138.7) for clean-up personnel to 138.2 (95% CI 138.0 to 138.5) for combat personnel, and were close to the ratio of 137.9 for natural uranium. The two highest individual ratios (146.9 and 147.7) were retested using more accurate, multiple collector inductively coupled plasma-mass spectrometry (MC-ICP-MS) and found to be within measurement of error of that for natural uranium. There were no significant differences in isotope ratio between participants according to self-reported circumstances of potential depleted uranium exposure. Conclusions Based on measurements using a SF-ICP-MS apparatus, this study provides reassurance following concern for potential widespread depleted uranium uptake in the UK military. The rare occurrence of elevated ratios may reflect the limits of accuracy of the SF-ICP-MS apparatus and not a real increase from the natural proportions of the isotopes. Any uptake of depleted uranium among participants in this study sample would be

  6. A stable isotope and fluid inclusion study of minor Upper Mississipi Valley-type sulfide mineralization in Iowa, Illinois, and Wisconsin

    SciTech Connect

    Kutz, K.B.

    1988-07-01

    The Upper Mississippi Valley (UMV) zinc-lead district, one of the largest mining districts in the United States, is surrounded by a broad zone of minor base metal mineralization which encompasses approximately 100,000 km/sup 2/ in northwest Illinois, eastern Iowa, and southwest Wisconsin. Over 60 minor base metal occurrences of possible UMV type have been recognized in the outlying zone. However, a genetic link between the outlying mineralization and the ore deposits of the main UMV district has not been firmly established. Although many of the outlying mineral occurrences exhibit close similarities to the main UMV ore deposits, paragenetic, fluid inclusion, and stable isotope (S, C, O, and H) data suggest major differences in the genetic history of the outlying occurrences.

  7. U235: a gamma ray analysis code for uranium isotopic determination

    SciTech Connect

    Clark, D.

    1997-12-01

    A {sup 235}U analysis code, U235, has been written that can nondestructively determine the percentage of {sup 235}U in a uranium sample from the analysis of the emitted gamma rays. The code is operational and work is now underway to improve the accuracy of the calculation, particularly at the high (>90%) and low (<0.7%) {sup 235}U concentrations. A technique has been found to evaluate low {sup 235}U concentrations that works well on the existing standards. Work is now under way to evaluate this technique for other detectors and other types of samples. Work is also proceeding on: (1) ways to better determine gamma backgrounds, (2) techniques to determine the equivalent thickness of the sample to correct for gamma attenuation, (3) evaluation of the existing data base of branching ratios of {sup 235}U, {sup 238}U and their daughters gamma rays to allow better results and (4) evaluation of the existing data base on the emission ratios for uranium, thorium, and protactinium x-rays.

  8. Coupled uranium isotope and sea-level variations in the oceans

    NASA Astrophysics Data System (ADS)

    Esat, Tezer M.; Yokoyama, Yusuke

    2010-12-01

    Globally, rivers supply uranium to the oceans with excess 234U relative to secular equilibrium and 234U taken-up by corals can be used for dating. In addition, the 234U abundance in sea water, at the time the coral was growing, can be measured independently. The veracity of U-series ages used in determining past sea-level variations is dependent on selecting pristine corals free from diagenetic alteration. A quantitative test for alteration assumes invariant 234U abundances in the oceans for at least the past half a million years and results from samples outside of a narrow range in modern ocean 234U abundance are excluded from data sets. Here, we have used previously published data to show that 234U in the oceans appears to be variable and directly related to changes in sea-level, not only over long glacial-interglacial timescales but also at very short, centennial timescales. Most of the previously discarded data can be used to provide valuable additional sea-level information. The process permits a unique insight into the interplay between sources and sinks of uranium in the oceans mediated by sea-level changes at rates far faster than previously thought possible. Similar, rapid sea-level, forcing of other trace element abundances in the oceans is likely.

  9. Assumptions and Criteria for Performing a Feasability Study of the Conversion of the High Flux Isotope Reactor Core to Use Low-Enriched Uranium Fuel

    SciTech Connect

    Primm, R.T., III; Ellis, R.J.; Gehin, J.C.; Moses, D.L.; Binder, J.L.; Xoubi, N.

    2006-02-01

    A computational study will be initiated during fiscal year 2006 to examine the feasibility of converting the High Flux Isotope Reactor from highly enriched uranium fuel to low-enriched uranium. The study will be limited to steady-state, nominal operation, reactor physics and thermal-hydraulic analyses of a uranium-molybdenum alloy that would be substituted for the current fuel powder--U{sub 3}O{sub 8} mixed with aluminum. The purposes of this document are to (1) define the scope of studies to be conducted, (2) define the methodologies to be used to conduct the studies, (3) define the assumptions that serve as input to the methodologies, (4) provide an efficient means for communication with the Department of Energy and American research reactor operators, and (5) expedite review and commentary by those parties.

  10. Geochemical, isotopic, and geochronlologic constraints on the formation of the Eagle Point basement-hosted uranium deposit, Athabasca Basin, Saskatchewan, Canada and recent remobilization of primary uraninite in secondary structures

    NASA Astrophysics Data System (ADS)

    Cloutier, Jonathan; Kyser, Kurt; Olivo, Gema R.; Brisbin, Dan

    2011-01-01

    The Athabasca Basin hosts many world-class unconformity-related uranium deposits. Recently, uranium reserves for the Eagle Point basement-hosted deposit have increased with the discovery of new mineralized zones within secondary structures. A paragenetic study of Eagle Point reveals the presence of three temporally distinct alteration stages: a pre-Athabasca alteration, a main alteration and mineralization comprised of three substages, and a post-main alteration and mineralization stage that culminated in remobilization of uraninite from primary to secondary structures. The pre-Athabasca alteration stage consists of minor amounts of clinochlore, followed by dolomite and calcite alteration in the hanging wall of major fault zones and kaolinitization of plagioclase and K-feldspar caused by surface weathering. The main alteration and uranium mineralization stage is related to three temporally distinct substages, all of which were produced by isotopically similar fluids. A major early alteration substage characterized by muscovite alteration and by precipitation Ca-Sr-LREE-rich aluminum phosphate-sulfate minerals, both from basinal fluids at temperatures around 240°C prior to 1,600 Ma. The mineralization substage involved uraninite and hematite precipitated in primary structures. The late alteration substage consists of dravite, uranophane-beta veins, calcite veins, and sudoite alteration from Mg-Ca-rich chemically modified basinal fluids with temperatures around 180°C. The post-main alteration and mineralization stage is characterized by remobilization of main stage uraninite from primary to secondary structures at a minimum age of ca. 535 Ma. U-Pb resetting events recorded on primary and remobilized uraninites are coincident with fluid flow induced by distal orogenies, remobilizing radiogenic Pb to a distance of at least 225 m above the mineralized zones.

  11. Utilization of non-weapons-grade plutonium and highly enriched uranium with breeding of the {sup 233}U isotope in the VVER reactors using thorium and heavy water

    SciTech Connect

    Marshalkin, V. E. Povyshev, V. M.

    2015-12-15

    A method for joint utilization of non-weapons-grade plutonium and highly enriched uranium in the thorium–uranium—plutonium oxide fuel of a water-moderated reactor with a varying water composition (D{sub 2}O, H{sub 2}O) is proposed. The method is characterized by efficient breeding of the {sup 233}U isotope and safe reactor operation and is comparatively simple to implement.

  12. [Determination of 235U/238U isotope ratios in camphor tree bark samples by MC-ICP-MS after separation of uranium from matrix elements].

    PubMed

    Wang, Xiao-Ping; Zhang, Ji-Long

    2007-07-01

    Twelve camphor (cinnamomum camphora) tree bark samples were collected from Hiroshima and Kyoto, and the matrix element composition and morphology of the outer surface of these camphor tree bark samples were studied by EDXS and SEM respectively. After a dry decomposition, DOWEX 1-X8 anion exchange resin was used to separate uranium from matrix elements in these camphor tree bark samples. Finally, 235U/238 U isotope ratios in purified uranium solutions were determined by MC-ICP-MS. It was demonstrated that the outer surface of these camphor tree bark samples is porous and rough, with Al, Ca, Fe, K, Mg, Si, C, O and S as its matrix element composition. Uranium in these camphor tree bark samples can be efficiently separated and quantitatively recovered from the matrix element composition. Compared with those collected from Kyoto, the camphor tree bark samples collected from Hiroshima have significantly higher uranium contents, which may be due to the increased aerosol mass concentration during the city reconstruction. Moreover, the 235 U/23.U isotope ratios in a few camphor tree bark samples collected from Hiroshima are slightly higher than 0.007 25. PMID:17944430

  13. Environmental site description for a Uranium Atomic Vapor Laser Isotope Separation (U-AVLIS) production plant at the Paducah Gaseous Diffusion Plant site

    SciTech Connect

    Marmer, G.J.; Dunn, C.P.; Moeller, K.L.; Pfingston, J.M.; Policastro, A.J.; Yuen, C.R.; Cleland, J.H.

    1991-09-01

    Uranium enrichment in the United States has utilized a diffusion process to preferentially enrich the U-235 isotope in the uranium product. The U-AVLIS process is based on electrostatic extraction of photoionized U-235 atoms from an atomic vapor stream created by electron-beam vaporization of uranium metal alloy. The U-235 atoms are ionized when precisely tuned laser light -- of appropriate power, spectral, and temporal characteristics -- illuminates the uranium vapor and selectively photoionizes the U-235 isotope. A programmatic document for use in screening DOE site to locate a U-AVLIS production plant was developed and implemented in two parts. The first part consisted of a series of screening analyses, based on exclusionary and other criteria, that identified a reasonable number of candidate sites. These sites were subjected to a more rigorous and detailed comparative analysis for the purpose of developing a short list of reasonable alternative sites for later environmental examination. This environmental site description (ESD) provides a detailed description of the PGDP site and vicinity suitable for use in an environmental impact statement (EIS). The report is based on existing literature, data collected at the site, and information collected by Argonne National Laboratory (ANL) staff during a site visit. 65 refs., 15 tabs.

  14. Determination of trace element concentrations and stable lead, uranium and thorium isotope ratios by quadrupole-ICP-MS in NORM and NORM-polluted sample leachates.

    PubMed

    Mas, J L; Villa, M; Hurtado, S; García-Tenorio, R

    2012-02-29

    This work focuses on the monitoring of the potential pollution in scenarios that involve NORM-related industrial activities (environmental or in-door scenarios). The objective was to develop a method to determine extent and origin of the contamination, suitable for monitoring (i.e. simple, fast and economical) and avoiding the use of too many different instruments. It is presented a radiochemical method that allows the determination of trace element concentrations and 206Pb/207Pb/208Pb, 238U/234U and 232Th/230Th isotope ratios using a single sample aliquot and a single instrument (ICP-QMS). Eichrom UTEVA® extraction chromatography minicolumns were used to separate uranium and thorium in sample leachates. Independent ICP-MS determinations of uranium and thorium isotope ratios were carried out afterwards. Previously a small aliquot of the leachate was used for the determination of trace element concentrations and lead isotope ratios. Several radiochemical arrangements were tested to get maximum performances and simplicity of the method. The performances of the method were studied in terms of chemical yields of uranium and thorium and removal of the potentially interfering elements. The established method was applied to samples from a chemical industry and sediments collected in a NORM-polluted scenario. The results obtained from our method allowed us to infer not only the extent, but also the sources of the contamination in the area. PMID:22230754

  15. Study of Fission Barrier Heights of Uranium Isotopes by the Macroscopic-Microscopic Method

    NASA Astrophysics Data System (ADS)

    Zhong, Chun-Lai; Fan, Tie-Shuan

    2014-09-01

    Potential energy surfaces of uranium nuclei in the range of mass numbers 229 through 244 are investigated in the framework of the macroscopic-microscopic model and the heights of static fission barriers are obtained in terms of a double-humped structure. The macroscopic part of the nuclear energy is calculated according to Lublin—Strasbourg-drop (LSD) model. Shell and pairing corrections as the microscopic part are calculated with a folded-Yukawa single-particle potential. The calculation is carried out in a five-dimensional parameter space of the generalized Lawrence shapes. In order to extract saddle points on the potential energy surface, a new algorithm which can effectively find an optimal fission path leading from the ground state to the scission point is developed. The comparison of our results with available experimental data and others' theoretical results confirms the reliability of our calculations.

  16. Reference (Axially Graded) Low Enriched Uranium Fuel Design for the High Flux Isotope Reactor (HFIR)

    SciTech Connect

    Ilas, Germina; Primm, Trent

    2010-01-01

    During the past five years, staff at the Oak Ridge National Laboratory (ORNL) have studied the issue of whether the HFIR could be converted to low enriched uranium (LEU) fuel without degrading the performance of the reactor. Using state-of-the-art reactor physics methods and behind-the-state-of-the-art thermal hydraulics methods, the staff have developed fuel plate designs (HFIR uses two types of fuel plates) that are believed to meet physics and thermal hydraulic criteria provided the reactor power is increased from 85 to 100 MW. The paper will present a defense of the results by explaining the design and validation process. A discussion of the requirements for showing applicability of analyses to approval for loading the fuel to HFIR lead test core irradiation currently scheduled for 2016 will be provided. Finally, the potential benefits of upgrading thermal hydraulics methods will be discussed.

  17. Uranium series isotopes concentration in sediments at San Marcos and Luis L. Leon reservoirs, Chihuahua, Mexico

    SciTech Connect

    Méndez-García, C.; Montero-Cabrera, M. E.; Renteria-Villalobos, M.; García-Tenorio, R.

    2008-01-01

    Spatial and temporal distribution of the radioisotopes concentrations were determined in sediments near the surface and core samples extracted from two reservoirs located in an arid region close to Chihuahua City, Mexico. At San Marcos reservoir one core was studied, while from Luis L. Leon reservoir one core from the entrance and another one close to the wall were investigated. ²³²Th-series, ²³⁸U-series, ⁴⁰K and ¹³⁷Cs activity concentrations (AC, Bq kg⁻¹) were determined by gamma spectrometry with a high purity Ge detector. ²³⁸U and ²³⁴U ACs were obtained by liquid scintillation and alpha spectrometry with a surface barrier detector. Dating of core sediments was performed applying CRS method to ²¹⁰Pb activities. Results were verified by ¹³⁷Cs AC. Resulting activity concentrations were compared among corresponding surface and core sediments. High ²³⁸U-series AC values were found in sediments from San Marcos reservoir, because this site is located close to the Victorino uranium deposit. Low AC values found in Luis L. Leon reservoir suggest that the uranium present in the source of the Sacramento – Chuviscar Rivers is not transported up to the Conchos River. Activity ratios (AR) ²³⁴U/²³⁸U and ²³⁸U/²²⁶Ra in sediments have values between 0.9–1.2, showing a behavior close to radioactive equilibrium in the entire basin. ²³²Th/²³⁸U, ²²⁸Ra/²²⁶Ra ARs are witnesses of the different geological origin of sediments from San Marcos and Luis L. Leon reservoirs.

  18. Uranium series isotopes concentration in sediments at San Marcos and Luis L. Leon reservoirs, Chihuahua, Mexico

    NASA Astrophysics Data System (ADS)

    Méndez-García, C.; Renteria-Villalobos, M.; García-Tenorio, R.; Montero-Cabrera, M. E.

    2014-07-01

    Spatial and temporal distribution of the radioisotopes concentrations were determined in sediments near the surface and core samples extracted from two reservoirs located in an arid region close to Chihuahua City, Mexico. At San Marcos reservoir one core was studied, while from Luis L. Leon reservoir one core from the entrance and another one close to the wall were investigated. 232Th-series, 238U-series, 40K and 137Cs activity concentrations (AC, Bq kg-1) were determined by gamma spectrometry with a high purity Ge detector. 238U and 234U ACs were obtained by liquid scintillation and alpha spectrometry with a surface barrier detector. Dating of core sediments was performed applying CRS method to 210Pb activities. Results were verified by 137Cs AC. Resulting activity concentrations were compared among corresponding surface and core sediments. High 238U-series AC values were found in sediments from San Marcos reservoir, because this site is located close to the Victorino uranium deposit. Low AC values found in Luis L. Leon reservoir suggest that the uranium present in the source of the Sacramento - Chuviscar Rivers is not transported up to the Conchos River. Activity ratios (AR) 234U/overflow="scroll">238U and 238U/overflow="scroll">226Ra in sediments have values between 0.9-1.2, showing a behavior close to radioactive equilibrium in the entire basin. 232Th/overflow="scroll">238U, 228Ra/overflow="scroll">226Ra ARs are witnesses of the different geological origin of sediments from San Marcos and Luis L. Leon reservoirs.

  19. Isotope-Geochmical Evidence For Uranium Retardation in Zeolitized Tuffs at Yucca Mountain, Nevada, USA

    SciTech Connect

    L.A. Neymark; J.B. Paces

    2007-02-14

    Retardation of radionuclides by sorption on minerals in the rocks along downgradient groundwater flow paths is a positive attribute of the natural barrier at Yucca Mountain, Nevada, the site of a proposed high-level nuclear waste repository. Alteration of volcanic glass in nonwelded tuffs beneath the proposed repository horizon produced thick, widespread zones of zeolite- and clay-rich rocks with high sorptive capacities. The high sorptive capacity of these rocks is enhanced by the large surface area of tabular to fibrous mineral forms, which is about 10 times larger in zeolitic tuffs than in devitrified tuffs and about 30 times larger than in vitric tuffs. The alteration of glass to zeolites, however, was accompanied by expansion that reduced the matrix porosity and permeability. Because water would then flow mainly through fractures, the overall effectiveness of radionuclide retardation in the zeolitized matrix actually may be decreased relative to unaltered vitric tuff. Isotope ratios in the decay chain of {sup 238}U are sensitive indicators of long-term water-rock interaction. In systems older than about 1 m.y. that remain closed to mass transfer, decay products of {sup 238}U are in secular radioactive equilibrium where {sup 234}U/{sup 238}U activity ratios (AR) are unity. However, water-rock interaction along flow paths may result in radioactive disequilibrium in both the water and the rock, the degree of which depends on water flux, rock dissolution rates, {alpha}-recoil processes, adsorption and desorption, and the precipitation of secondary minerals. The effects of long-term water-rock interaction that may cause radionuclide retardation were measured in samples of Miocene-age subrepository zeolitized tuffs of the Calico Hills Formation (Tac) and the Prow Pass Tuff (Tcp) from borehole USW SD-9 near the northern part of the proposed repository area (sampled depth interval from 451.1 to 633.7 m; Engstrom and Rautman, 1996). Mineral abundances and whole

  20. Uranium isotopic distribution in the mineral phases of granitic fracture fillings by a sequential extraction procedure.

    PubMed

    Crespo, M T; Pérez del Villar, L; Jiménez, A; Pelayo, M; Quejido, A; Sánchez, M

    1996-01-01

    In order to study the recent rock-water interaction processes in the E1 Berrocal site, a sequential leaching method has been applied to granitic fracture fillings to obtain the U isotopic distribution in the mineral phases of these samples. Based on the mineralogical composition of these materials, six dissolution steps have been chosen to extract U as exchangeable cation, from carbonates, amorphous Fe-oxyhydroxides, labile resistates and highly insoluble resistates. In this way, the processes involved in the rock-water interaction phenomena, mainly dissolution, precipitation, coprecipitation and adsorption can be distinguished and even approximately dated. PMID:8976044

  1. Flow-injection technique for determination of uranium and thorium isotopes in urine by inductively coupled plasma mass spectrometry.

    PubMed

    Benkhedda, Karima; Epov, Vladimir N; Evans, R Douglas

    2005-04-01

    A sensitive and efficient flow-injection (FI) preconcentration and matrix-separation technique coupled to sector field ICP-mass spectrometry (SF-ICP-MS) has been developed and validated for simultaneous determination of ultra-low levels of uranium (U) and thorium (Th) in human urine. The method is based on selective retention of U and Th from a urine matrix, after microwave digestion, on an extraction chromatographic TRU resin, as an alternative to U/TEVA resin, and their subsequent elution with ammonium oxalate. Using a 10 mL sample, the limits of detection achieved for 238U and 232Th were 0.02 and 0.03 ng L(-1), respectively. The accuracy of the method was checked by spike-recovery measurements. Levels of U and Th in human urine were found to be in the ranges 1.86-5.50 and 0.176-2.35 ng L(-1), respectively, well in agreement with levels considered normal for non-occupationally exposed persons. The precision obtained for five replicate measurements of a urine sample was 2 and 3% for U and Th, respectively. The method also enables on-line measurements of the 235U/238U isotope ratios in urine. Precision of 0.82-1.04% (RSD) was obtained for 235U/238U at low ng L(-1) levels, using the FI transient signal approach. PMID:15827719

  2. Measurement of uranium and plutonium in solid waste by passive photon or neutron counting and isotopic neutron source interrogation

    SciTech Connect

    Crane, T.W.

    1980-03-01

    A summary of the status and applicability of nondestructive assay (NDA) techniques for the measurement of uranium and plutonium in 55-gal barrels of solid waste is reported. The NDA techniques reviewed include passive gamma-ray and x-ray counting with scintillator, solid state, and proportional gas photon detectors, passive neutron counting, and active neutron interrogation with neutron and gamma-ray counting. The active neutron interrogation methods are limited to those employing isotopic neutron sources. Three generic neutron sources (alpha-n, photoneutron, and /sup 252/Cf) are considered. The neutron detectors reviewed for both prompt and delayed fission neutron detection with the above sources include thermal (/sup 3/He, /sup 10/BF/sub 3/) and recoil (/sup 4/He, CH/sub 4/) proportional gas detectors and liquid and plastic scintillator detectors. The instrument found to be best suited for low-level measurements (< 10 nCi/g) is the /sup 252/Cf Shuffler. The measurement technique consists of passive neutron counting followed by cyclic activation using a /sup 252/Cf source and delayed neutron counting with the source withdrawn. It is recommended that a waste assay station composed of a /sup 252/Cf Shuffler, a gamma-ray scanner, and a screening station be tested and evaluated at a nuclear waste site. 34 figures, 15 tables.

  3. Uranium-Series Isotopic Constraints on Recent Changes in the Eruptive Behaviour of Merapi Volcano, Java, Indonesia

    NASA Astrophysics Data System (ADS)

    Gertisser, R.; Handley, H. K.; Reagan, M. K.; Berlo, K.; Barclay, J.; Preece, K.; Herd, R.

    2011-12-01

    Merapi volcano (Central Java) is one of the most active and deadly volcanoes in Indonesia. The 2010 eruption was the volcano's largest eruption since 1872 and erupted much more violently than expected. Prior to 2010, volcanic activity at Merapi was characterised by several months of slow dome growth punctuated by gravitational dome failures, generating small-volume pyroclastic density currents (Merapi-type nuées ardentes). The unforeseen, large-magnitude events in 2010 were different in many respects: pyroclastic density currents travelled > 15 km beyond the summit causing widespread devastation in proximal areas on Merapi's south flank and ash emissions from sustained eruption columns resulted in ash fall tens of kilometres away from the volcano. The 2010 events have proved that Merapi's relatively small dome-forming activity can be interrupted at relatively short notice by larger explosive eruptions, which appear more common in the geological record. We present new geochemical and Uranium-series isotope data for the volcanic products of both the 2006 and 2010 eruptions at Merapi to investigate the driving forces behind this unusual explosive behaviour and their timescales. An improved knowledge of these processes and of changes in the pre-eruptive magma system has important implications for the assessment of hazards and risks from future eruptive activity at Merapi.

  4. Distribution of uranium and radium isotopes in an aquifer of a semi-arid region (Manouba-Essijoumi, Northern Tunisia).

    PubMed

    Added, A; Ben Mammou, A; Fernex, F; Rezzoug, S; Bernat, M

    2005-01-01

    Groundwaters from the Sebkhet Essijoumi drainage basin, situated in northern Tunisia, West of the city of Tunis, were sampled and analyzed for uranium and radium isotopes. Low (234)U/(238)U activity ratios coupled with relatively high (228)Ra and (238)U concentrations were found in the Manouba plain phreatic aquifer, at the northern part of the basin, where remote sensing has indicated that this plain corresponds to the main humid zone of the area. Low (234)U/(238)U ratios probably reflected short residence time for waters in the Manouba plain, and high ratios longer residence time in the south, where water reaching the phreatic aquifer seems to have previously circulated in rocks constituting the southern hills. Assuming that, in the Manouba plain aquifer, the groundwater flows downstream from the Oued Lill pass area to the South-West of the Sebkha, the difference in the (228)Ra/(226)Ra activity ratio suggests that the residence time of water has been 2.8 years longer near the Sebkha than upstream. PMID:15885382

  5. Late quaternary history and uranium isotopic compositions of ground water discharge deposits, Crater Flat, Nevada

    SciTech Connect

    Paces, J.B.; Taylor, E.M.; Bush, C.

    1993-12-31

    Three carbonate-rich spring deposits are present near the southern end of Crater Flat, NV, approximately 18 km southwest of the potential high-level waste repository at Yucca Mountain. We have analyzed five samples of carbonate-rich material from two of the deposits for U and Th isotopic compositions. Resulting U-series disequilibrium ages indicate that springs were active at 18 {+-} 1, 30 {+-} 3, 45 {+-} 4 and >70 ka. These ages are consistent with a crude internal stratigraphy at one site. Identical ages for two samples at two separate sites suggest that springs were contemporaneous, at least in part, and were most likely part of the same hydrodynamic system. In addition, initial U isotopic compositions range from 2.8 to 3.8 and strongly suggest that ground water from the regional Tertiary-volcanic aquifer provided the source for these hydrogenic deposits. This interpretation, along with water level data from near-by wells suggest that the water table rose approximately 80 to 115 m above present levels during the late Quaternary and may have fluctuated repeatedly. Current data are insufficient to allow reconstruction of a detailed depositional history, however geochronological data are in a good agreement with other paleoclimatic proxy records preserved throughout the region. Since these deposits are down gradient from the potential repository site, the possibility of higher ground water levels in the future dramatically shortens both vertical and lateral ground water pathways and reduces travel times of transported radionuclides to potential discharge sites.

  6. New Insights into Arctic Tectonics: Uranium-Lead, (Uranium-Thorium)/Helium, and Hafnium Isotopic Data from the Franklinian Basin, Canadian Arctic Islands

    NASA Astrophysics Data System (ADS)

    Anfinson, Owen Anthony

    More than 2300 detrital zircon uranium-lead (U-Pb) ages, 32 176Hf/177Hf (eHf) isotopic values, 37 apatite helium (AHe) ages, and 72 zircon helium (ZHe) ages represent the first in-depth geochronologic and thermochronologic study of Franklinian Basin strata in the Canadian Arctic and provide new insight on >500 M.y. of geologic history along the northern Laurentian margin (modern orientation). Detrital zircon U-Pb age data demonstrate that the Franklinian Basin succession is composed of strata with three distinctly different provenance signatures. Neoproterozoic and Lower Cambrian formations contain detrital zircon populations consistent with derivation from Archean to Paleoproterozoic gneisses and granites of the west Greenland--northeast Canadian Shield. Lower Silurian to Middle Devonian strata are primarily derived from foreland basin strata of the East Greenland Caledonides (Caledonian orogen). Middle Devonian to Upper Devonian strata also contain detrital zircon populations interpreted as being primarily northerly derived from the continental landmass responsible for the Ellesmerian Orogen (often referred to as Crockerland). U-Pb age data from basal turbidites of the Middle to Upper Devonian clastic succession suggest Crockerland contributed sediment to the northern Laurentian margin by early-Middle Devonian time and that prior to the Ellesmerian Orogeny Crockerland had a comparable geologic history to the northern Baltica Craton. Detrital zircon U-Pb ages in Upper Devonian strata suggest Crockerland became the dominant source by the end of Franklinian Basin sedimentation. Mean eHf values from Paleozoic detrital zircon derived from Crockerland suggest the zircons were primarily formed in either an island arc or continental arc built on accreted oceanic crust setting. ZHe cooling ages from Middle and Upper Devonian strata were not buried deeper than 7 km since deposition and suggest Crockerland was partially exhumed during the Caledonian Orogen. AHe cooling ages

  7. Uranium and Sm isotope studies of the supergiant Olympic Dam Cu-Au-U-Ag deposit, South Australia

    NASA Astrophysics Data System (ADS)

    Kirchenbaur, Maria; Maas, Roland; Ehrig, Kathy; Kamenetsky, Vadim S.; Strub, Erik; Ballhaus, Chris; Münker, Carsten

    2016-05-01

    The Olympic Dam Cu-U-Au-Ag deposit in the Archean-Proterozoic Gawler Craton (South Australia) is a type example of the iron oxide-copper-gold (IOCG) spectrum of deposits and one of the largest Cu-U-Au resources known. Mineralization is hosted in a lithologically and texturally diverse, hematite-rich breccia complex developed within a granite of the 1.59 Ga Gawler Silicic Province. Emerging evidence indicates that both the breccia complex and its metal content developed over ∼1000 Ma, responding to major tectonic events, e.g., at 1300-1100, 825 and 500 Ma. However, metal sources and exact mechanism/s of ore formation remain poorly known. New high-precision 238U/235U data for a set of 40 whole rock samples representing all major lithological facies of the breccia complex show a narrow range (δ238UCRM112a = -0.56‰ to +0.04‰). At the scale of sampling, there is no correlation of δ238U with lithology, degree of alteration or U mineralogy, although ores with U > 5 wt.% have subtly higher δ238U values (-0.20‰ to 0.00) than the majority of samples (<0.7 wt.% U, -0.56‰ to -0.23‰). The new U isotope data are consistent with published data for uraninites from Olympic Dam, and with published results from high-temperature U deposits. They overlap completely with the range of δ238U values in granitoids (including the host granite, -0.18‰ to -0.32‰) and with estimates of the upper continental crust in general. This similarity suggests that Olympic Dam δ238U values reflects the crustal sources of U, which probably include felsic volcanic rocks and granitoids. The isotopic homogeneity suggests depositional mechanisms that involve minimal isotopic fractionation of U; alternatively, primary fractionation signatures may have been erased during the long history of the U mineralization. High-grade U ores may record isotopic neutron-capture effects related to fissionogenic neutrons. High-precision Sm isotope data for five high-U (>5 wt.% U, U/Sm ≫ 500) Olympic Dam

  8. Determination of elemental impurities and U and O isotopic compositions with a view to identify the geographical and industrial origins of uranium ore concentrates

    NASA Astrophysics Data System (ADS)

    Salaun, A.; Hubert, A.; Pointurier, F.; Aupiais, J.; Pili, E.; Richon, P.; Fauré, A.; Diallo, S.

    2012-12-01

    First events of illicit trafficking of nuclear and radiological materials occurred 50 years ago. Nuclear forensics expertise are aiming at determining the use of seized material, its industrial history and provenance (geographical area, place of production or processing), at assisting in the identification and dismantling of illicit trafficking networks. This information is also valuable in the context of inspections of declared facilities to verify the consistency of operator's declaration. Several characteristics can be used to determine the origin of uranium ore concentrates such as trace elemental impurity patterns (Keegan et al., 2008 ; Varga et al., 2010a, 2010b) or uranium, oxygen and lead isotopic compositions (Tamborini et al., 2002a, 2002b ; Wallenius et al., 2006; Varga et al., 2009). We developed analytical procedures for measuring the isotopic compositions of uranium (234U/238U and 235U/238U) and oxygen (18O/16O) and levels of elemental impurities (e.g. REE, Th) from very small amounts of uranium ore concentrates (or yellow cakes). Micrometer particles and few milligrams of material are used for oxygen isotope measurements and REE determination, respectively. Reference materials were analyzed by mass spectrometry (TIMS, SF-ICP-MS and SIMS) to validate testing protocols. Finally, materials of unknown origin were analyzed to highlight significant differences and determine whether these differences allow identifying the origin of these ore concentrates. References: Keegan, E., et al. (2008). Applied Geochemistry 23, 765-777. Tamborini, G., et al. (2002a). Analytical Chemistry 74, 6098-6101. Tamborini, G., et al. (2002b). Microchimica Acta 139, 185-188. Varga, Z., et al. (2009). Analytical Chemistry 81, 8327-8334. Varga, Z., et al. (2010a). Talanta 80, 1744-1749. Varga, Z., et al. (2010b). Radiochimica Acta 98, 771-778 Wallenius, M., et al. (2006). Forensic Science International 156, 55-62.

  9. Melting of the Earth's lithospheric mantle inferred from protactinium-thorium-uranium isotopic data

    PubMed

    Asmerom; Cheng; Thomas; Hirschmann; Edwards

    2000-07-20

    The processes responsible for the generation of partial melt in the Earth's lithospheric mantle and the movement of this melt to the Earth's surface remain enigmatic, owing to the perceived difficulties in generating large-degree partial melts at depth and in transporting small-degree melts through a static lithosphere. Here we present a method of placing constraints on melting in the lithospheric mantle using 231Pa-235U data obtained from continental basalts in the southwestern United States and Mexico. Combined with 230Th-238U data, the 231Pa-235U data allow us to constrain the source mineralogy and thus the depth of melting of these basalts. Our analysis indicates that it is possible to transport small melt fractions--of the order of 0.1%--through the lithosphere, as might result from the coalescence of melt by compaction owing to melting-induced deformation. The large observed 231Pa excesses require that the timescale of melt generation and transport within the lithosphere is small compared to the half-life of 231Pa (approximately 32.7 kyr). The 231Pa-230Th data also constrain the thorium and uranium distribution coefficients for clinopyroxene in the source regions of these basalts to be within 2% of one another, indicating that in this setting 230Th excesses are not expected during melting at depths shallower than 85 km. PMID:10917528

  10. The geochemistry of uranium and thorium isotopes in the Western Desert of Egypt

    SciTech Connect

    Dabous, A.A.

    1994-11-01

    The concentrations of {sup 238}U, {sup 234}U, {sup 232}Th, and {sup 228}Th have been measured in the groundwaters of the Bahariya and Farafra oases of the Western Desert of Egypt. These waters are characterized by normal amounts of U, but unusually high concentrations of Th. The pattern of variation of the parent isotopes, {sup 238}U and {sup 232}Th, as well as the daughter isotopes, {sup 234}U, {sup 230}Th, and {sup 228}Th, is systematic within and between the two oases. From the unusually consistent distribution of the {sup 234}U/{sup 238}U activity ratios one can conclude that the samples from both oases are representative of a two-component mixing system. One component, characterized by low U content and a high {sup 234}U/{sup 238}U activity ratio, is typical of deep artesian systems and probably represents flowthrough water derived from the Nubian highlands to the south. The second component is characterized by a greater U concentration and a low activity ratio. This signature is hypothesized as being derived by leaching of downward infiltrating water during pluvial times. The source of the U may be the uraniferous phosphate strata that overly the sandstone aquifer in both oasis areas. Higher Th values are associated with the artesian flow component of the mixing system and suggests that Th-bearing minerals may be abundant in the Nubian sandstone aquifer. The distribution of {sup 230}Th and {sup 228}Th in the water samples supports this interpretation.

  11. Nuclear Isotopic Dilution of Highly-Enriched Uranium-235 and Uranium-233 by Dry Blending via the RM-2 Mill Technology

    SciTech Connect

    N. A. Chipman; R. N. Henry; R. K. Rajamani; S. Latchireddi; V. Devrani; H. Sethi; J. L. Malhotra

    2004-02-01

    The United States Department of Energy has initiated numerous activities to identify strategies to disposition various excess fissile materials. Two such materials are the off-specification highly enriched uranium-235 oxide powder and the uranium-233 contained in unirradiated nuclear fuel both currently stored at the Idaho National Engineering and Environmental Laboratory. This report describes the development of a technology that could dilute these materials to levels categorized as low-enriched uranium, or further dilute the materials to a level categorized as waste. This dilution technology opens additional pathways for the disposition of these excess fissile materials as existing processing infrastructure continues to be retired.

  12. Isotopes of uranium and thorium, lead-210, and polonium-210 in the lungs of coal miners of Appalachia and the lungs and livers of residents of central Ohio

    SciTech Connect

    Gilbert, G.E.; Casella, V.R.; Bishop, C.T.; Aguirre, A.G.

    1985-10-21

    The lungs of twelve and the livers of three residents of central Ohio and the lungs of four coal miners of Appalachia were analyzed for uranium-238, uranium-234, thorium-230, lead-210, polonium-210, and thorium-232. Mean and median lung concentrations of uranium-238 and of uranium-234 in the lungs of central Ohioans were essentially the same and were equal to 4 fCi/g dry. Mean concentrations of these isotopes in the lungs of Appalachian coal miners were also essentially the same and were equal to 9 fCi/g. Little uranium was found in the liver. The median concentration of thorium-230 in the lungs of central Ohioans was also 4 fCi/g dry; however, the mean concentration was 8 fCi/g due to the relatively high concentration values in a few persons. The mean concentrations of this isotope in the lungs of central Ohioans and Appalachian coal miners were essentially the same; i.e. 8 fCi/g. The mean and median concentrations of thorium-232 in the lungs of central Ohioans were assentially the same and equal to 4 fCi/g. The mean concentration of this isotope in the lungs of Appalachian coal miners was 9 fCi/g. Little thorium was found in the liver. The mean concentrations of lead-210 in the lungs of the two populations were nearly equal and about 23 fCi/g dry. The mean liver/lung ratio of this isotope was essentially two, and the concentrations appeared to be positively correlated with smoking. Polonium-210 concentrations in the lungs were distributed into three sets of values which are described here as low (2-4 fCi/g), medium (20-30 fCi/g), and high (>100 fCi/g), and also appeared to be correlated with smoking. Mean liver concentrations of this irotope were nearly equal to the mean liver concentrations of lead-210 (50 as opposed to 47 fCi/g). 18 refs., 6 tabs.

  13. Measurement of Uranium Isotopes in Particles of U3O8 by Secondary Ion Mass Spectrometry-Single-Stage Accelerator Mass Spectrometry (SIMS-SSAMS).

    PubMed

    Fahey, Albert J; Groopman, Evan E; Grabowski, Kenneth S; Fazel, Kamron C

    2016-07-19

    A commercial secondary ion mass spectrometer (SIMS) was coupled to a ± 300 kV single-stage accelerator mass spectrometer (SSAMS). Positive secondary ions generated with the SIMS were injected into the SSAMS for analysis. This combined instrument was used to measure the uranium isotopic ratios in particles of three certified reference materials (CRM) of uranium, CRM U030a, CRM U500, and CRM U850. The ability to inject positive ions into the SSAMS is unique for AMS systems and allows for simple analysis of nearly the entire periodic table because most elements will readily produce positive ions. Isotopic ratios were measured on samples of a few picograms to nanograms of total U. Destruction of UH(+) ions in the stripper tube of the SSAMS reduced hydride levels by a factor of ∼3 × 10(4) giving the UH(+)/U(+) ratio at the SSAMS detector of ∼1.4 × 10(-8). These hydride ion levels would allow the measurement of (239)Pu at the 10 ppb level in the presence of U and the equivalent of ∼10(-10 236)U concentration in natural uranium. SIMS-SSAMS analysis of solid nuclear materials, such as these, with signals nearly free of molecular interferences, could have a significant future impact on the way some measurements are made for nuclear nonproliferation. PMID:27321905

  14. Microscopic description of fission in uranium isotopes with the Gogny energy density functional

    NASA Astrophysics Data System (ADS)

    Rodríguez-Guzmán, R.; Robledo, L. M.

    2014-05-01

    The most recent parametrizations D1S, D1N, and D1M of the Gogny energy density functional are used to describe fission in the isotopes 232-280U. Fission paths, collective masses, and zero-point quantum corrections, obtained within the constrained Hartree-Fock-Bogoliubov approximation, are used to compute the systematics of the spontaneous fission half-lives tSF, the masses and charges of the fission fragments, and their intrinsic shapes. The Gogny-D1M parametrization has been benchmarked against available experimental data on inner and second barrier heights, excitation energies of the fission isomers, and half-lives in a selected set of Pu, Cm, Cf, Fm, No, Rf, Sg, Hs, and Fl nuclei. It is concluded that D1M represents a reasonable starting point to describe fission in heavy and superheavy nuclei. Special attention is also paid to understand the uncertainties in the predicted tSF values arising from the different building blocks entering the standard semiclassical Wentzel-Kramers-Brillouin formula. Although the uncertainties are large, the trend with mass or neutron numbers are well reproduced and therefore the theory still has predictive power. In this respect, it is also shown that modifications of a few percent in the pairing strength can have a significant impact on the collective masses leading to uncertainties in the tSF values of several orders of magnitude.

  15. Conceptual Process for the Manufacture of Low-Enriched Uranium/Molybdenum Fuel for the High Flux Isotope Reactor

    SciTech Connect

    Sease, J.D.; Primm, R.T. III; Miller, J.H.

    2007-09-30

    The U.S. nonproliferation policy 'to minimize, and to the extent possible, eliminate the use of HEU in civil nuclear programs throughout the world' has resulted in the conversion (or scheduled conversion) of many of the U.S. research reactors from high-enriched uranium (HEU) to low-enriched uranium (LEU). A foil fuel appears to offer the best option for using a LEU fuel in the High Flux Isotope Reactor (HFIR) without degrading the performance of the reactor. The purpose of this document is to outline a proposed conceptual fabrication process flow sheet for a new, foil-type, 19.75%-enriched fuel for HFIR. The preparation of the flow sheet allows a better understanding of the costs of infrastructure modifications, operating costs, and implementation schedule issues associated with the fabrication of LEU fuel for HFIR. Preparation of a reference flow sheet is one of the first planning steps needed in the development of a new manufacturing capacity for low enriched fuels for U.S. research and test reactors. The flow sheet can be used to develop a work breakdown structure (WBS), a critical path schedule, and identify development needs. The reference flow sheet presented in this report is specifically for production of LEU foil fuel for the HFIR. The need for an overall reference flow sheet for production of fuel for all High Performance Research Reactors (HPRR) has been identified by the national program office. This report could provide a starting point for the development of such a reference flow sheet for a foil-based fuel for all HPRRs. The reference flow sheet presented is based on processes currently being developed by the national program for the LEU foil fuel when available, processes used historically in the manufacture of other nuclear fuels and materials, and processes used in other manufacturing industries producing a product configuration similar to the form required in manufacturing a foil fuel. The processes in the reference flow sheet are within the

  16. Redistribution of uranium and thorium series isotopes during isovolumetric weathering of granite

    NASA Astrophysics Data System (ADS)

    Michel, Jacqueline

    1984-06-01

    Previous studies of the distribution of U and Th in parent versus weathered granites have shown both depletion and enrichment of these elements during weathering. In this study, the distribution of U and Th decay series isotopes was determined in a weathering profile of a granitic saprolite, which showed textural preservation indicating isovolumetric weathering. Two types of dissolution methods were used: a whole-rock dissolution and a sodium-citrate dithionite leach to preferentially attack noncrystalline phases of weathering products. Using volume-based activities, 45-70 percent of the total 232Th was gradually removed during weathering. Although the whole-rock 228Th /232Th activity ratios were in equilibrium, there were large excesses of 228Th in the leachable fraction of both parent rock ( 228Th /232Th = 2.06 ) and partially weathered saprolite ( 228Th /232Th = 3-6.5 ), due to alpha recoil and release of daughter 228Th to the weathering rind of the mineral grain. For the most weathered sample, 81 percent of the thorium was in the teachable fraction and 228Th /232Th = 1 , indicating that even the more resistant minerals were attacked. The total U activities showed as much variation in the six parent rock samples as in the weathered profile, and 234U /238U were in equilibrium in both the whole-rock and leachable fractions. 230Th was deficient relative to 234U and 226Ra in both fractions, suggesting recent addition of U and Ra to the entire profile. The large variation in U was not from absorption onto the intermediate weathering products, because only 11-23 percent of the U was in the leachable fraction.

  17. Towards A Modern Calibration Of The 238U/235U Paleoredox Proxy: Apparent Uranium Isotope Fractionation Factor During U(VI)-U(IV) Reduction In The Black Sea

    NASA Astrophysics Data System (ADS)

    Rolison, J. M.; Stirling, C. H.; Middag, R.; Rijkenberg, M. J. A.; De Baar, H. J. W.

    2015-12-01

    The isotopic compositions of redox-sensitive metals, including uranium (U), in marine sediments have recently emerged as powerful diagnostic tracers of the redox state of the ancient ocean-atmosphere system. Interpretation of sedimentary isotopic information requires a thorough understating of the environmental controls on isotopic fractionation in modern anoxic environments before being applied to the paleo-record. In this study, the relationship between ocean anoxia and the isotopic fractionation of U was investigated in the water column and sediments of the Black Sea. The Black Sea is the world's largest anoxic basin and significant removal of U from the water column and high U accumulation rates in modern underlying sediments have been documented. Removal of U from the water column occurs during the redox transition of soluble U(VI) to relatively insoluble U(IV). The primary results of this study are two-fold. First, significant 238U/235U fractionation was observed in the water column of the Black Sea, suggesting the reduction of U induces 238U/235U fractionation with the preferential removal of 238U from the aqueous phase. Second, the 238U/235U of underlying sediments is related to the water column through the isotope fractionation factor of the reduction reaction but is influenced by mass transport processes. These results provide important constraints on the use of 238U/235U as a proxy of the redox state of ancient oceans.

  18. Borate Exchanges of Lemna minor L. as Studied with the Help of the Enriched Stable Isotopes and of a (n,α) Nuclear Reaction 1

    PubMed Central

    Thellier, Michel; Duval, Yves; Demarty, Maurice

    1979-01-01

    Despite the lack of a convenient radioisotope of boron, it is possible to measure unidirectional fluxes of borate between cellular systems and their external medium. It was accomplished by using the two purified stable isotopes (10B and 11B), with 10B specifically detected by a (n,α) nuclear reaction. The method was applied to compartmental analysis of borate with intact plants of Lemna minor L. Four compartments were suggested. Three of them apparently correspond to the three classical ones: free space (including easily dissociable borate monoesters), cytoplasm, and vacuole. The fourth one was interpreted as corresponding to very stable borate diesters in the cell walls. The method allows the determination of the borate capacities of the various compartments and of the borate unidirectional fluxes between the different compartments, at borate flux equilibrium. Other physicochemical data (mono and diester mass action constants, turn over numbers) were evaluated. The results are consistent with what is known of pure substances. PMID:16660714

  19. The Development of Low-Level Measurement Capabilities for Total and Isotopic Uranium in Environmental Samples at Brazilian and Argentine Laboratories by ABACC

    SciTech Connect

    Guidicini, Olga M.; Olsen, Khris B.; Hembree, Doyle M.; Carter, Joel A.; Whitaker, Michael; Hayes, Susan M.

    2005-07-01

    In June 1998, the Brazilian-Argentine Agency for Accounting and Control of Nuclear Materials (ABACC), with assistance from the U.S. Department of Energy (DOE), began a program to assess environmental sampling and analysis capabilities at laboratories in Argentina and Brazil. The program began with staff training conducted in South America and the United States by Oak Ridge National Laboratory (ORNL) and Pacific Northwest National Laboratory (PNNL). Both laboratories are participating members of DOE’s Network of Analytical Laboratories (NWAL) that support IAEA’s environmental sampling program. During the initial planning meeting, representatives from ABACC and all the participating analytical laboratories supporting ABACC were briefed on how the first exercise would be managed and on key aspects necessary to analyze low-level environmental samples for uranium. Subsequent to this training, a laboratory evaluation exercise (Exercise 1) was conducted using standard swipe samples prepared for this exercise by the International Atomic Energy Agency (IAEA). The results of Exercise 1 determined that sample contamination was a major factor in the analysis, and a thorough review of laboratory procedures was required to reduce the level of contamination to acceptable levels. Following modification of sample preparation procedures, the laboratories performed Exercise 2, an analysis of a National Institute of Standards and Technology (NIST) Standard Reference Material (SRM) 1547, Peach Leaves. The results of Exercise 2 demonstrated that several laboratories were capable of accurately determining the total uranium and uranium isotopic distribution in the peach leaves. To build on these successes, Exercise 3 was performed using a series of standard swipe samples prepared by the IAEA and distributed to laboratories supporting ABACC and to PNNL and ORNL. The results of Exercise 3 demonstrate that ABACC now has support laboratories in both Argentina and Brazil, which are capable

  20. Uranium-isotope disequilibrium in brine reservoirs of the Castile Formation, northern Delaware Basin, southeastern New Mexico. I. Principles and methods

    SciTech Connect

    Lambert, S.J.; Carter, J.A.

    1984-02-01

    We evaluated uranium isotope activity ratios with respect to models for the origin of the brines in two brine reservoirs in the Castile Formation (ERDA No. 6 and WIPP No. 12). In Castile anhydrite, a completely closed water system that was continuously leaching Th-recoil-produced /sup 234/U from freshly exposed surfaces of fractured host rock would give rise to uranium 234/238 isotope activity ratio (..cap alpha..) values significantly higher than observed values. Therefore, the brine occurrences are not the result of continuous deformation. Similarly, a model assuming movement of intergranular Permian seawater into fractures was found inconsistent with observed uranium isotope systematics. The observed ..cap alpha..-values (95% confidence limits) of ERDA No. 6 (1.34 to 1.58) and WIPP No. 12 (1.74 to 2.54), used in conjunction with an inferred intial ..cap alpha../sub 0/ higher than observed values, allows calculation of reasonable finite minimum ages, involving no preferential leaching of /sup 234/U in the host rock. If the brine occurrences are inferred to have been connected at one time with a more extensive nearby hydrologic system, the Capitan limestone (..cap alpha../sub 0/ = 5.1), calculated minimum ages of isolation from that system are 700,000 to 880,000 yr for ERDA No. 6 and 360,000 to 610,000 yr for WIPP No. 12. These ranges in ages are the 95% confidence limits based on experimental determinations of ..cap alpha..-values. The ages thus derived may reflect an episode of structural deformation in the Pleistocene that allowed water to enter the resulting fractures. 16 references, 6 figures.

  1. Modeling non-steady state radioisotope transport in the vadose zone--A case study using uranium isotopes at Pena Blanca, Mexico

    SciTech Connect

    Ku, T. L.; Luo, S.; Goldstein, S. J.; Murrell, M. T.; Chu, W. L.; Dobson, P. F.

    2009-06-01

    Current models using U- and Th-series disequilibria to study radioisotope transport in groundwater systems mostly consider a steady-state situation. These models have limited applicability to the vadose zone (UZ) where the concentration and migratory behavior of radioisotopes in fluid are often transitory. We present here, as a first attempt of its kind, a model simulating the non-steady state, intermittent fluid transport in vadose layers. It provides quantitative constraints on in-situ migration of dissolved and colloidal radioisotopes in terms of retardation factor and rock-water interaction (or water transit) time. For uranium, the simulation predicts that intermittent flushing in the UZ leads to a linear relationship between reciprocal U concentration and {sup 234}U/{sup 238}U ratio in percolating waters, with the intercept and slope bearing information on the rates of dissolution and {alpha}-recoil of U isotopes, respectively. The general validity of the model appears to be borne out by the measurement of uranium isotopes in UZ waters collected at various times over a period during 1995-2006 from a site in the Pena Blanca mining district, Mexico, where the Nopal I uranium deposit is located. Enhanced {sup 234}U/{sup 238}U ratios in vadose-zone waters resulting from lengthened non-flushing time as prescribed by the model provide an interpretative basis for using {sup 234}U/{sup 238}U in cave calcites to reconstruct the regional changes in hydrology and climate. We also provide a theoretical account of the model's potential applications using radium isotopes.

  2. Modeling non-steady state radioisotope transport in the vadose zone - A case study using uranium isotopes at Peña Blanca, Mexico

    NASA Astrophysics Data System (ADS)

    Ku, T. L.; Luo, S.; Goldstein, S. J.; Murrell, M. T.; Chu, W. L.; Dobson, P. F.

    2009-10-01

    Current models using U- and Th-series disequilibria to study radioisotope transport in groundwater systems mostly consider a steady-state situation. These models have limited applicability to the vadose zone (UZ) where the concentration and migratory behavior of radioisotopes in fluid are often transitory. We present here, as a first attempt of its kind, a model simulating the non-steady state, intermittent fluid transport in vadose layers. It provides quantitative constraints on in-situ migration of dissolved and colloidal radioisotopes in terms of retardation factor and rock-water interaction (or water transit) time. For uranium, the simulation predicts that intermittent flushing in the UZ leads to a linear relationship between reciprocal U concentration and 234U/ 238U ratio in percolating waters, with the intercept and slope bearing information on the rates of dissolution and α-recoil of U isotopes, respectively. The general validity of the model appears to be borne out by the measurement of uranium isotopes in UZ waters collected at various times over a period during 1995-2006 from a site in the Peña Blanca mining district, Mexico, where the Nopal I uranium deposit is located. Enhanced 234U/ 238U ratios in vadose-zone waters resulting from lengthened non-flushing time as prescribed by the model provide an interpretative basis for using 234U/ 238U in cave calcites to reconstruct the regional changes in hydrology and climate. We also provide a theoretical account of the model's potential applications using radium isotopes.

  3. Uranium-lead isotopic ages from the Sierra Nevada Batholith, California

    NASA Astrophysics Data System (ADS)

    Chen, James H.; Moore, James G.

    1982-06-01

    all in the range 99±3 m.y., indicating a relatively short period of emplacement and cooling for this nested group of plutons. U-Pb ages of a mafic inclusion and its host granodiorite indicate that both were derived from a common source or that the mafic inclusion was totally equilibrated with the granodioritic magma. Comparison of isotopic ages determined by different methods such as zircon U-Pb, sphene U-Pb, hornblende K-Ar, and biotite K-Ar suggests that zircon U-Pb ages generally approximate the emplacement age of a pluton. However, some plutons probably contain inherited or entrained old zircons, and the zircons of some samples are disturbed by younger thermal and metamorphic events. The ages reported here are consistent with U-Pb age determinations previously made on granitic rocks to the north [Stern et al., 1981], The age distribution of granitic belts determined here is in general agreement with those established by K-Ar dating [Evernden and Kistler, 1970] but does not differentiate the five epochs of plutonism determined in their study.

  4. Hydrologic and climatic implications of stable isotope and minor element analyses of authigenic calcite silts and gastropod shells from a mid-Pleistocene pluvial lake, Western Desert, Egypt

    NASA Astrophysics Data System (ADS)

    Kieniewicz, Johanna M.; Smith, Jennifer R.

    2007-11-01

    Authigenic calcite silts at Wadi Midauwara in Kharga Oasis, Egypt, indicate the prolonged presence of surface water during the Marine Isotope Stage 5e pluvial phase recognized across North Africa. Exposed over an area of ˜ 4.25 km 2, these silts record the ponding of water derived from springs along the Libyan Plateau escarpment and from surface drainage. The δ 18O values of these lacustrine carbonates (- 11.3‰ to - 8.0‰ PDB), are too high to reflect equilibrium precipitation with Nubian aquifer water or water of an exclusively Atlantic origin. Mg/Ca and Sr/Ca of the silts have a modest negative covariance with silt δ 18O values, suggesting that the water may have experienced the shortest residence time in local aquifers when the water δ 18O values were highest. Furthermore, intra-shell δ 18O, Sr/Ca, and Ba/Ca analyses of the freshwater gastropod Melanoides tuberculata are consistent with a perennially fresh water source, suggesting that strong evaporative effects expected in a monsoonal climate did not occur, or that dry season spring flow was of sufficient magnitude to mute the effects of evaporation. The input of a second, isotopically heavier water source to aquifers, possibly Indian Ocean monsoonal rain, could explain the observed trends in δ 18O and minor element ratios.

  5. Trace and minor element variations and sulfur isotopes in crystalline and colloform ZnS: Incorporation mechanisms and implications for their genesis

    USGS Publications Warehouse

    Pfaff, Katharina; Koenig, Alan; Wenzel, Thomas; Ridley, Ian; Hildebrandt, Ludwig H.; Leach, David L.; Markl, Gregor

    2011-01-01

    Various models have been proposed to explain the formation mechanism of colloform sphalerite, but the origin is still under debate. In order to decipher influences on trace element incorporation and sulfur isotope composition, crystalline and colloform sphalerite from the carbonate-hosted Mississippi-Valley Type (MVT) deposit near Wiesloch, SW Germany, were investigated and compared to sphalerite samples from 52 hydrothermal vein-type deposits in the Schwarzwald ore district, SW Germany to study the influence of different host rocks, formation mechanisms and fluid origin on trace element incorporation. Trace and minor element incorporation in sphalerite shows some correlation to their host rock and/or origin of fluid, gangue, paragenetic minerals and precipitation mechanisms (e.g., diagenetic processes, fluid cooling or fluid mixing). Furthermore, crystalline sphalerite is generally enriched in elements like Cd, Cu, Sb and Ag compared to colloform sphalerite that mainly incorporates elements like As, Pb and Tl. In addition, sulfur isotopes are characterized by positive values for crystalline and strongly negative values for colloform sphalerite. The combination of trace element contents, typical minerals associated with colloform sphalerite from Wiesloch, sulfur isotopes and thermodynamic considerations helped to evaluate the involvement of sulfate-reducing bacteria in water-filled karst cavities. Sulfate-reducing bacteria cause a sulfide-rich environment that leads in case of a metal-rich fluid supply to a sudden oversaturation of the fluid with respect to galena, sphalerite and pyrite. This, however, exactly coincides with the observed crystallization sequence of samples involving colloform sphalerite from the Wiesloch MVT deposit.

  6. Preparation, certification and validation of a stable solid spike of uranium and plutonium coated with a cellulose derivative for the measurement of uranium and plutonium content in dissolved nuclear fuel by isotope dilution mass spectrometry.

    PubMed

    Surugaya, Naoki; Hiyama, Toshiaki; Verbruggen, André; Wellum, Roger

    2008-02-01

    A stable solid spike for the measurement of uranium and plutonium content in nitric acid solutions of spent nuclear fuel by isotope dilution mass spectrometry has been prepared at the European Commission Institute for Reference Materials and Measurements in Belgium. The spike contains about 50 mg of uranium with a 19.838% (235)U enrichment and 2 mg of plutonium with a 97.766% (239)Pu abundance in each individual ampoule. The dried materials were covered with a thin film of cellulose acetate butyrate as a protective organic stabilizer to resist shocks encountered during transportation and to eliminate flaking-off during long-term storage. It was found that the cellulose acetate butyrate has good characteristics, maintaining a thin film for a long time, but readily dissolving on heating with nitric acid solution. The solid spike containing cellulose acetate butyrate was certified as a reference material with certified quantities: (235)U and (239)Pu amounts and uranium and plutonium amount ratios, and was validated by analyzing spent fuel dissolver solutions of the Tokai reprocessing plant in Japan. This paper describes the preparation, certification and validation of the solid spike coated with a cellulose derivative. PMID:18270417

  7. Improving Precision and Accuracy of Isotope Ratios from Short Transient Laser Ablation-Multicollector-Inductively Coupled Plasma Mass Spectrometry Signals: Application to Micrometer-Size Uranium Particles.

    PubMed

    Claverie, Fanny; Hubert, Amélie; Berail, Sylvain; Donard, Ariane; Pointurier, Fabien; Pécheyran, Christophe

    2016-04-19

    The isotope drift encountered on short transient signals measured by multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) is related to differences in detector time responses. Faraday to Faraday and Faraday to ion counter time lags were determined and corrected using VBA data processing based on the synchronization of the isotope signals. The coefficient of determination of the linear fit between the two isotopes was selected as the best criterion to obtain accurate detector time lag. The procedure was applied to the analysis by laser ablation-MC-ICPMS of micrometer sized uranium particles (1-3.5 μm). Linear regression slope (LRS) (one isotope plotted over the other), point-by-point, and integration methods were tested to calculate the (235)U/(238)U and (234)U/(238)U ratios. Relative internal precisions of 0.86 to 1.7% and 1.2 to 2.4% were obtained for (235)U/(238)U and (234)U/(238)U, respectively, using LRS calculation, time lag, and mass bias corrections. A relative external precision of 2.1% was obtained for (235)U/(238)U ratios with good accuracy (relative difference with respect to the reference value below 1%). PMID:27031645

  8. Uranium isotopes as a potential global-ocean redox proxy: a test from the Upper Pennsylvanian Hushpuckney Shale (Kansas, U.S.A.)

    NASA Astrophysics Data System (ADS)

    Herrmann, A. D.; Algeo, T. J.; Gordon, G. W.; Anbar, A. D.

    2015-12-01

    Uranium (U) isotope variation in marine sediments has been proposed as a proxy for changes in average global-ocean redox conditions. Here, we investigate U isotope variation in the black shale (BS) member of the Hushpuckney Shale (Swope Formation) at two sites ~400 km apart within the Late Paleozoic Midcontinent Sea (LPMS) of North America, with the goal of testing whether sediment δ238U records a global-ocean redox signal or local environmental influences. Our results document a spatial gradient of at least 0.25‰ in δ238U within the LPMS, demonstrating that local (probably redox) controls have overprinted any global U-isotope signal. Furthermore, the pattern of stratigraphic variation in δ238U in both study cores, with low values (‒0.4 to ‒0.2‰) at the base and top and peak values (+0.4 to +0.65‰) in the middle of the BS, is inconsistent with dominance of a global-ocean redox signal because (1) the middle of the BS was deposited at maximum eustatic highstand when euxinic conditions existed most widely within the LPMS and coeval epicontinental seas, and (2) more extensive euxinia should have shifted global-ocean seawater δ238U to lower values based on mass-balance principles. On the other hand, the observed δ238U pattern is consistent with a dominant local redox control, with larger U-isotope fractionations associated with more reducing bottom waters. We therefore conclude that U was not removed quantitatively to euxinic facies of the LPMS, and that sediment U-isotope compositions were controlled mainly by local redox and hydrographic factors. Our results imply that U-isotope signals from epicontinental-sea sections must be vetted carefully through analysis of high-resolution datasets at multiple sites in order to validate their potential use as a global-seawater redox proxy.

  9. Accurate fast method with high chemical yield for determination of uranium isotopes (234U, 235U, 238U) in granitic samples using alpha spectroscopy

    NASA Astrophysics Data System (ADS)

    Guirguis, Laila A.; Farag, Nagdy M.; Salim, Adham K.

    2015-03-01

    The present study aims to use the α-spectroscopy at Nuclear Materials Authority (NMA) of Egypt. A radiochemical technique for analysis uranium isotopes was carried out for ten mineralized granitic samples together with the International standards RGU-1 (IAEA) and St4 (NMA). Several steps of sample preparation, radiochemical separation and source preparation were performed before analysis. Uranium was separated from sample matrix with 0.2 M TOPO in cyclohexane as an extracting agent with a chemical yield 98.95% then uranium was purified from lanthanides and actinides present with 0.2 M TOA in xylene as an extracting agent. The pure fraction was electrodeposited on a mirror-polished copper disc from buffer solution (NaHSO4+H2SO4+NH4OH). Rectangle pt-electrode with an anode-cathode distance of 2 cm was used. Current was 900 mA and the electrodeposition time reach up to 120 min. The achieved results show that the chemical yield ranged between 87.9±6.8 and 98±8.6.

  10. Cross section generation and physics modeling in a feasibility study of the conversion of the high flux isotope reactor core to use low-enriched uranium fuel

    SciTech Connect

    Ellis, R. J.; Gehin, J. C.; Primm Iii, R. T.

    2006-07-01

    A computational study has been initiated at ORNL to examine the feasibility of converting the High Flux Isotope Reactor (HFIR) from highly enriched uranium (HEU) fuel to low-enriched uranium (LEU) fuel. The current study is limited to steady-state, nominal operation and are focused on the determination of the fuel requirements, primarily density, that are required to maintain the performance of the reactor. Reactor physics analyses are reported for a uranium-molybdenum alloy that would be substituted for the current fuel - U{sub 3}O{sub 8} mixed with aluminum. An LEU core design has been obtained and requires an increase in {sup 235}U loading of a factor of 1.9 over the current HEU fuel. These initial results indicate that the conversion from HEU to LEU results in a reduction of the thermal fluxes in the central flux trap region of approximately 9 % and in the outer beryllium reflector region of approximately 15%. Ongoing work is being performed to improve upon this initial design to further minimize the impact of conversion to LEU fuel. (authors)

  11. Preliminary Assessment of the Impact on Reactor Vessel dpa Rates Due to Installation of a Proposed Low Enriched Uranium (LEU) Core in the High Flux Isotope Reactor (HFIR)

    SciTech Connect

    Daily, Charles R.

    2015-10-01

    An assessment of the impact on the High Flux Isotope Reactor (HFIR) reactor vessel (RV) displacements-per-atom (dpa) rates due to operations with the proposed low enriched uranium (LEU) core described by Ilas and Primm has been performed and is presented herein. The analyses documented herein support the conclusion that conversion of HFIR to low-enriched uranium (LEU) core operations using the LEU core design of Ilas and Primm will have no negative impact on HFIR RV dpa rates. Since its inception, HFIR has been operated with highly enriched uranium (HEU) cores. As part of an effort sponsored by the National Nuclear Security Administration (NNSA), conversion to LEU cores is being considered for future HFIR operations. The HFIR LEU configurations analyzed are consistent with the LEU core models used by Ilas and Primm and the HEU balance-of-plant models used by Risner and Blakeman in the latest analyses performed to support the HFIR materials surveillance program. The Risner and Blakeman analyses, as well as the studies documented herein, are the first to apply the hybrid transport methods available in the Automated Variance reduction Generator (ADVANTG) code to HFIR RV dpa rate calculations. These calculations have been performed on the Oak Ridge National Laboratory (ORNL) Institutional Cluster (OIC) with version 1.60 of the Monte Carlo N-Particle 5 (MCNP5) computer code.

  12. Combining U speciation and U isotope fractionation to evaluate the importance of naturally reduced sediments in controlling the mobility of uranium in the upper Colorado River Basin

    NASA Astrophysics Data System (ADS)

    Noel, V.; Lefebvre, P.; Boye, K.; Bargar, J.; Maher, K.; Lezama-Pacheco, J.; Cardarelli, E.; Bone, S.; Dam, W. L.; Johnson, R. H.

    2015-12-01

    Long-term persistence of uranium (U) in groundwater at legacy ore-processing sites in the upper Colorado River Basin (CRB) is a major concern for DOE, stakeholders, and local property owners. In the past year, we have investigated U distributions in contaminated floodplains at Grand Junction, Naturita, and Rifle (CO), Riverton (WY), and Shiprock (NM). We find that U is retained at all locations in fine-grained, organic-rich sulfidic sediments, referred to as naturally reduced zones (NRZs). The retention mechanisms (e.g., complexation, precipitation or adsorption) and the processes responsible for U accumulation in NRZs will directly determine the capacity of the sediments to prevent U mobilization. However, these processes remain poorly understood at local and regional scales yet they are critical to management and remediation of these sites. We have used U LIII/II-edge XANES to systematically characterize U oxidation states, and EXAFS and bicarbonate extractions to characterize U local structure and reactivity in order to distinguish the forms of U. We are measuring U isotopic signatures (δ238/235U) to better understand uranium sources and processes of accumulation in NRZs. We have found that high U concentrations correspond to reduced and relatively insoluble U forms, mainly non-crystalline U(IV), and co-occur with ferrous iron and sulfides. This suggests that reduction processes, fueled by the high organic matter content and constrained to the diffusion-limited environment in the fine-grained NRZs, are important for the retention of U in these sediments. We also observe a strong correlation between the U concentrations in the NRZs and the extent of isotopic fractionation, with up to +1.8 ‰ difference between uranium-enriched and low concentration zones. In some locations the δ238/235U values are within the range of values typical of the mine tailings, whereas at other sites the more positive δ238/235U values suggest that redox cycling and/or partial

  13. Environmental site description for a Uranium Atomic Vapor Laser Isotope Separation (U-AVLIS) production plant at the Portsmouth Gaseous Diffusion Plant site

    SciTech Connect

    Marmer, G.J.; Dunn, C.P.; Filley, T.H.; Moeller, K.L.; Pfingston, J.M.; Policastro, A.J.; Cleland, J.H.

    1991-09-01

    Uranium enrichment in the United States has utilized a diffusion process to preferentially enrich the U-235 isotope in the uranium product. In the 1970s, the US Department of Energy (DOE) began investigating more efficient and cost-effective enrichment technologies. In January 1990, the Secretary of Energy approved a plan for the demonstration and deployment of the Uranium Atomic Vapor Laser isotope Separation (U-AVLIS) technology with the near-term goal to provide the necessary information to make a deployment decision by November 1992. Initial facility operation is anticipated for 1999. A programmatic document for use in screening DOE sites to locate a U-AVLIS production plant was developed and implemented in two parts. The first part consisted of a series of screening analyses, based on exclusionary and other criteria, that identified a reasonable number of candidate sites. The final evaluation, which included sensitivity studies, identified the Oak Ridge Gaseous Diffusion Plant (ORGDP) site, the Paducah Gaseous Diffusion Plant (PGDP) site, and the Portsmouth Gaseous Diffusion Plant (PORTS) site as having significant advantages over the other sites considered. This environmental site description (ESD) provides a detailed description of the PORTS site and vicinity suitable for use in an environmental impact statement (EIS). This report is based on existing literature, data collected at the site, and information collected by Argonne National Laboratory (ANL) staff during site visits. The organization of the ESD is as follows. Topics addressed in Sec. 2 include a general site description and the disciplines of geology, water resources, biotic resources, air resources, noise, cultural resources, land use. Socioeconomics, and waste management. Identification of any additional data that would be required for an EIS is presented in Sec. 3.

  14. Secondary ion mass spectrometry combined with alpha track detection for isotope abundance ratio analysis of individual uranium-bearing particles.

    PubMed

    Esaka, Fumitaka; Magara, Masaaki

    2014-03-01

    Secondary ion mass spectrometry (SIMS) was used in combination with alpha track detection for the efficient analysis of uranium-bearing particles with higher (235)U abundances in environmental samples. A polycarbonate film containing particles was prepared and placed in contact with a CR-39 plastic detector. After exposure for 28 days, the detector was etched in a NaOH solution and each uranium-bearing particle was identified through observation of the alpha tracks recorded in the detector. A portion of the film containing each uranium-bearing particle was cut out and put onto a glassy carbon planchet. The films on the planchet were decomposed through plasma ashing for subsequent uranium abundance ratio analysis with SIMS. The alpha track-SIMS analysis of 10 uranium-bearing particles in a sample taken from a nuclear facility enabled n((235)U)/n((238)U) abundance ratios in the range 0.0072-0.25 to be detected, which were significantly higher than those obtained by SIMS without alpha track detection. The duration of the whole analytical process for analysis of 10 particles was about 32 days. The detection efficiency was calculated to be 27.1±6.5%, based on the analysis of the particles in uranium reference materials. The detection limits, defined as the diameter of the particle which produces alpha tracks more than one for a 28-days exposure, were estimated to be 0.8, 0.9, 1.1, 2.1 and 3.0 μm for the particles having the same uranium abundance ratios with NBL CRM U850, U500, U350, U050 and U010 reference materials, respectively. The use of alpha track detection for subsequent SIMS analysis is an inexpensive and an efficient way to measure uranium-bearing particles with higher (235)U abundances. PMID:24468381

  15. Chemistry, spectroscopy, and isotope-selective infrared photochemistry of volatile uranium compound tailored for 10-. mu. m absorption: U(OCH/sub 3/)/sub 6/

    SciTech Connect

    Cuellar, E.A.; Miller, S.S.; Marks, T.J.; Weitz, E.

    1983-07-13

    This contribution reports on the chemical, vibrational spectroscopic, and infrared multiphoton photochemical properties of uranium hexamethoxide, U(OCH/sub 3/)/sub 6/, a prototype molecule for laser-induced uranium isotope separation with a carbon dioxide laser. Uranium hexamethoxide can be prepared from UCl/sub 4/ by conversion to Li/sub 2/U(OCH/sub 3/)/sub 6/, followed by oxidation with lead tetraacetate. Vapor pressure studies on U(OCH/sub 3/)/sub 6/ indicate that at 33/sup 0/C, the vapor pressure is 17 mtorr. The vibrational spectra of U(/sup 16/OCH/sub 3/)/sub 6/ and U(/sup 18/OCH/sub 3/)/sub 6/ have been assigned by using infrared and laser Raman data. Under idealized O/sub h/ symmetry, the U(/sup 16/OCH/sub 3/)/sub 6/ U-O stretching fundamentals are assigned at 505.0 (A/sub lg/), 464.8(T/sub 1u/, and 414.0 cm/sup -1/ (E/sub g/). Tentative assignments are also made for several of the overtone and combination transitions evidence for possible lowering of the symmetry is presented. In gas-phase infrared photochemical experiments, the predominant U(OCH/sub 3/)/sub 6/ photoproducts isolated are U(OCH/sub 3/)/sub 5/, methanol, and formaldhyde. These are suggestive of multiphoton U-O bond homolysis to produce uranium pentamethoxide and methoxy radicals. The enrichment of unreacted U(OCH/sub 3/)/sub 6/ in /sup 235/U is maximum at ca 927 cm/sup -1/ (near what may be a U-O stretching overtone transition) and exhibits both a low fluence threshold and diminution at high fluence.

  16. Chemistry, spectroscopy, and isotope-selective infrared photochemistry of a volatile uranium compound tailored for 10-mm absorption: U(OCH/sub 3/)/sub 6/

    SciTech Connect

    Cuellar, E.A.; Miller, S.S.; Marks, T.J.; Weitz, E.

    1983-07-13

    This contribution reports on the chemical, vibrational spectroscopic, and infrared multiphoton photochemical properties of uranium hexamethoxide, U(OCH/sub 3/)/sub 6/, a prototype molecule for laser-induced uranium isotope separation with a carbon dioxide laser. Uranium hexamethoxide can be prepared from UCl/sub 4/ by conversion to Li/sub 2/U(OCH/sub 3/)/sub 6/, followed by oxidation with lead tetraacetate. Vapor pressure studies on U(OCH/sub 3/)/sub 6/ indicate that ..delta..H/sub sub//sup 0/ = 23 +/- 3 kcal/mol and ..delta..S/sub sub//sup 0/ = 76 +/- 4 eu; at 33/sup 0/C, the vapor pressure is 17 mtorr. The vibrational spectra of U(/sup 16/OCH/sub 3/)/sub 6/ and U(/sup 18/OCH/sub 3/)/sub 6/ have been assigned by using infrared and laser Raman data. Under idealized O/sub h/ symmetry, the U(/sup 16/OCH/sub 3/)/sub 6/U-O stretching fundamentals are assigned at 505.0 (A/sub 1g/), 464.8 (T/sub 1u/), and 414.0 cm/sup -1/ (E/sub g/). Tentative assignments are also made for several of the overtone and combination transitions evidence for possible lowering of the symmetry is presented. In gas-phase infrared photochemical experiments, the predominant U(OCH/sub 3/)/sub 6/ photoproducts isolated are U(OCH/sub 3/)/sub 5/, methanol, and formaldehyde. These are suggestive of multiphoton U-O bond homolysis to produce uranium pentamethoxide and methoxy radicals. The enrichment of unreacted U(OCH/sub 3/)/sub 6/ in /sup 235/U is maximum at ca. 927 cm/sup -1/ (near what may be a U-O stretching overtone transition) and exhibits both a low fluence threshold and dimunution at high fluence.

  17. Uranium-lead isotopic ages of the Samail ophiolite, Oman, with applicatons to Tethyan ocean ridge tectonics

    SciTech Connect

    Tilton, G.R.; Hopson, C.A.; Wright, J.E.

    1981-04-10

    Plagiogranites are a minor but widespread component of the Samail ophiolite plutonic member. They crystallized from the most fractionated melts generated by magmatic crystallization and differentiation of a steady state magma chamber beneath the Tethyan spreading ocean ridge, and their ages are thought to mark the time of ocean crust formation. Isotopic U--Pb ages of zircons from 13 plagiogranites collected along a 270-km segment of the Samail ophiolite subparallel to the regional trend of the sheeted dike complex (the former spreading ridge axis direction) define a narrow time interval of 93.5--97.9 m.y., with a pronounced clustering about 95 m.y. The zircon ages of the plagiogranites agree remarkably well with the early Cenomanian to early Turonian biostratigraphic ages of sediments that are intercalated within the ophiolite pillow lavas and that lie just above them (Tippit et al., 1981). The agreement of radiometric and biostratigraphic ages provides strong support for the conclusion that the plagiogranite U--Pb ages closely date the time span of ocean crust formation. No step changes in age patterns are observed along the ridge axis (sheeted dike) direction, suggesting that there are no major internal offsets of the ophiolite by transform or other faults along most of the traverse. One possible exception occurs at the southeastern end of the sampled interval (Ibra area), where a 3 m.y. discontinuity might be caused by an unmapped fault. Assuming that the regional trend of the sheeted dikes (N10 /sup 0/--25 /sup 0/W) marks the direction of the former spreading ridge axis, the present array of sample localities spans a distance of 130 to 195 km normal to that axis (i.e., in the spreading direction). The data as a whole do not define a clear-cut age trend normal to the spreading axis, but by eliminating samples that may be aberrant due to faulting, the data array suggests a pattern of increasing ages from east to west.

  18. Uranium series disequilibrium in a Holocene uranium deposit in northeastern Washington

    SciTech Connect

    Zielinski, R.A.; Bush, C.A.; Rosholt, J.N.

    1985-01-01

    A recently discovered ore-grade accumulation of uranium in post-glacial, organic-rich sediments provides an opportunity for studying the early association of uranium and organic matter in a natural setting. The uranium occurs in valley-fill sediments of peat, peaty clay, silt, and sand along the north fork of Flodelle Creek, Stevens County, Washington. Sixteen lithologically distinct intervals in a 290 cm core were measured by high-resolution gamma-ray spectrometry and by thin-source alpha spectrometry to determine the abundance and distribution of uranium series nuclides and the extent of secular equilibrium within the uranium decay series. Samples taken above the 6700 to 7000 year old Mazama Ash (0-127 cm depth) are clearly most deficient in daughters, but a simple increase of daughters relative to uranium as a function of depth was not observed, probably because chemically diverse daughters that are decay-generated in situ have differing mobilities, and because upwelling ground waters continuously add more uranium and minor amounts of daughters. Measured alpha activity ratios of /sup 234/U//sup 238/U (1.31-1.38) are analytically indistinguishable from those measured in coexisting waters, suggesting a rather constant isotopic composition of introduced uranium and little preferential recoil of /sup 234/U daughter from sediment surfaces. A consistent excess of /sup 210/Pb relative to /sup 226/Ra is observed throughout the core, suggesting ground-water input of the highly mobile intervening daughter, /sup 222/Rn. The abundance of uranium (160-3300 ppm) correlates highly with the abundance of organic matter (3-60 wt.%) as do abundances of /sup 226/Ra, /sup 230/Th, and /sup 210/Pb below 127 cm depth.

  19. High-precision measurements of uranium and thorium isotopic ratios by multi-collector inductively coupled plasma mass spectrometry (MC-ICPMS)

    NASA Astrophysics Data System (ADS)

    Wang, Lisheng; Ma, Zhibang; Duan, Wuhui

    2015-04-01

    Isotopic compositions of U-Th and 230Th dating have been widely used in earth sciences, such as chronology, geochemistry, oceanography and hydrology. In this study, five ages of different carbonate samples were measured using 230Th dating technique with U-Th high-precision isotopic measurements by multi-collector inductively coupled plasma mass spectrometry, in Uranium-series Chronology Laboratory, Institute of Geology and Geophysics, Chinese Academy of Sciences.In this study, the precision and accuracy of uranium isotopic composition were estimated by measuring the uranium ratios of NBS-CRM 112A, NBS-CRM U500 and HU-1. The mean measured ratios, 234U/238U = 52.86 (±0.04) × 10-6 and δ234U = -38.36 (±0.77) × 10-3 for NBS-CRM 112A, 234U/238U = 10.4184 (±0.0001) × 10-3, 236U/238U = 15.43 (±0.01) × 10-4 and 238U/235U = 1.00021 (±0.00002) for NBS-CRM U500, 234U/238U = 54.911 (±0.007) and δ234U = -1.04 (±0.13) × 10-3 for HU-1 (95% confidence levels). The U isotope data for standard reference materials are in excellent agreement with previous studies, further highlighting the reliability and analytical capabilities of our technique. We measured the thorium isotopic ratios of three different thorium standards by MC-ICPMS. The three standards (Th-1, Th-2 and Th-3) were mixed by HU-1 and NBS 232Th standard, with the 230Th/232Th ratios from 10-4 to 10-6. The mean measured atomic ratios, 230Th/232Th = 2.1227 (±0.0024) × 10-6, 2.7246 (±0.0026) × 10-5, and 2.8358 (±0.0007) × 10-4 for Th-1, Th-2 and Th-3 (95% confidence levels), respectively. Using this technique, the following standard samples were dated by MC-ICPMS. Sample RKM-4, collected from Babardos Kendal Hill terrace, was used during the first stage of the Uranium-Series Intercomparison Project (USIP-I). Samples 76001, RKM-5 and RKM-6 were studied during the second stage of the USIP program (USIP-II). Sample 76001 is a laminated flowstone, collected from Sumidero Terejapa, Chiapas, Mexico, and samples

  20. Iron, zinc, magnesium and uranium isotopic fractionation during continental crust differentiation: The tale from migmatites, granitoids, and pegmatites

    NASA Astrophysics Data System (ADS)

    Telus, Myriam; Dauphas, Nicolas; Moynier, Frédéric; Tissot, François L. H.; Teng, Fang-Zhen; Nabelek, Peter I.; Craddock, Paul R.; Groat, Lee A.

    2012-11-01

    The causes of some stable isotopic variations in felsic rocks are not well understood. In particular, the origin of the heavy Fe isotopic compositions (i.e., high δ56Fe values, deviation in ‰ of the 56Fe/54Fe ratio relative to IRMM-014) of granites with SiO2 > 70 wt.% compared with less silicic rocks is still debated. It has been interpreted to reflect isotopic fractionation during late stage aqueous fluid exsolution, magma differentiation, partial melting, or Soret (thermal) diffusion. The present study addresses this issue by comparing the Fe isotopic compositions of a large range of differentiated crustal rocks (whole rocks of migmatites, granitoids, and pegmatites; mineral separates) with the isotopic compositions of Zn, Mg and U. The samples include granites, migmatites and pegmatites from the Black Hills, South Dakota (USA), as well as I-, S-, and A-type granitoids from Lachlan Fold Belt (Australia). The nature of the protolith (i.e., I- or S-type) does not influence the Fe isotopic composition of granitoids. Leucosomes (partial melts in migmatites) tend to have higher δ56Fe values than melanosomes (melt residues) indicating that partial melting of continental crust material can possibly fractionate Fe isotopes. No clear positive correlation is found between the isotopic compositions of Mg, U and Fe, which rules out the process of Soret diffusion in the systems studied here. Zinc isotopes were measured to trace fluid exsolution because Zn can easily be mobilized by aqueous fluids as chloride complexes. Pegmatites and some granitic rocks with high δ56Fe values also have high δ66Zn values. In addition, high-SiO2 granites show a large dispersion in the Zn/Fe ratio that cannot easily be explained by magma differentiation alone. These results suggest that fluid exsolution is responsible for some of the Fe isotopic fractionation documented in felsic rocks and in particular in pegmatites. However, some granites with high δ56Fe values have unfractionated δ66

  1. Predicting 232U Content in Uranium

    SciTech Connect

    AJ Peurrung

    1999-01-07

    The minor isotope 232U may ultimately be used for detection or confirmation of uranium in a variety of applications. The primary advantage of 232 U as an indicator of the presence of enriched uranium is the plentiful and penetrating nature of the radiation emitted by its daughter radionuclide 208Tl. A possible drawback to measuring uranium via 232U is the relatively high uncertainty in 232U abundance both within and between material populations. An important step in assessing this problem is to ascertain what determines the 232U concentration within any particular sample of uranium. To this end, we here analyze the production and eventual enrichment of 232 U during fuel-cycle operations. The goal of this analysis is to allow approximate prediction of 232 U quantities, or at least some interpretation of the results of 232U measurements. We have found that 232U is produced via a number of pathways during reactor irradiation of uranium and is subsequently concentrated during the later enrichment of the uranium' s 235U Content. While exact calculations are nearly impossible for both the reactor-production and cascade-enrichment parts of the prediction problem, estimates and physical bounds can be provided as listed below and detailed within the body of the report. Even if precise calculations for the irradiation and enrichment were possible, the ultimate 212U concentration would still depend upon the detailed fuel-cycle history. Assuming that a thennal-diffusion cascade is used to produce highly enriched uranium (HEU), dilution of reactor-processed fuel at the cascade input and the long-term holdup of 232U within the cascade both affect the 232U concentration in the product. Similar issues could be expected to apply for the other isotope-separation technologies that are used in other countries. Results of this analysis are listed below: 0 The 232U concentration depends strongly on the uranium enrichment, with depleted uranium (DU) containing between 1600 and 8000 times

  2. Minor Actinides Recycling in PWRs

    SciTech Connect

    Delpech, M.; Golfier, H.; Vasile, A.; Varaine, F.; Boucher, L.; Greneche, D.

    2006-07-01

    Recycling of minor actinides in current and near future PWR is considered as one of the options of the general waste management strategy. This paper presents the analysis of this option both from the core physics and fuel cycle point of view. A first indicator of the efficiency of different neutron spectra for transmutation purposes is the capture to fission cross sections ratio which is less favourable by a factor between 5 to 10 in PWRs compared to fast reactors. Another indicator presented is the production of high ranking isotopes like Curium, Berkelium or Californium in the thermal or epithermal spectrum conditions of PWR cores by successive neutron captures. The impact of the accumulation of this elements on the fabrication process of such PWR fuels strongly penalizes this option. The main constraint on minor actinides loadings in PWR (or fast reactors) fuels are related to their direct impact (or the impact of their transmutation products) on the reactivity coefficients, the reactivity control means and the core kinetics parameters. The main fuel cycle physical parameters like the neutron source, the alpha decay power, the gamma and neutrons dose rate and the criticality aspects are also affected. Recent neutronic calculations based on a reference core of the Evolutionary Pressurized Reactor (EPR), indicates typical maximum values of 1 % loadings. Different fuel design options for minor actinides transmutation purposes in PWRs are presented: UOX and MOX, homogeneous and heterogeneous assemblies. In this later case, Americium loading is concentrated in specific pins of a standard UOX assembly. Recycling of Neptunium in UOX and MOX fuels was also studied to improve the proliferation resistance of the fuel. The impact on the core physics and penalties on Uranium enrichment were underlined in this case. (authors)

  3. Natural uranium and strontium isotope tracers of water sources and surface water-groundwater interactions in arid wetlands - Pahranagat Valley, Nevada, USA

    NASA Astrophysics Data System (ADS)

    Paces, James B.; Wurster, Frederic C.

    2014-09-01

    Near-surface physical and chemical process can strongly affect dissolved-ion concentrations and stable-isotope compositions of water in wetland settings, especially under arid climate conditions. In contrast, heavy radiogenic isotopes of strontium (87Sr/86Sr) and uranium (234U/238U) remain largely unaffected and can be used to help identify unique signatures from different sources and quantify end-member mixing that would otherwise be difficult to determine. The utility of combined Sr and U isotopes are demonstrated in this study of wetland habitats on the Pahranagat National Wildlife Refuge, which depend on supply from large-volume springs north of the Refuge, and from small-volume springs and seeps within the Refuge. Water budgets from these sources have not been quantified previously. Evaporation, transpiration, seasonally variable surface flow, and water management practices complicate the use of conventional methods for determining source contributions and mixing relations. In contrast, 87Sr/86Sr and 234U/238U remain unfractionated under these conditions, and compositions at a given site remain constant. Differences in Sr- and U-isotopic signatures between individual sites can be related by simple two- or three-component mixing models. Results indicate that surface flow constituting the Refuge's irrigation source consists of a 65:25:10 mixture of water from two distinct regionally sourced carbonate-aquifer springs, and groundwater from locally sourced volcanic aquifers. Within the Refuge, contributions from the irrigation source and local groundwater are readily determined and depend on proximity to those sources as well as water management practices.

  4. Natural uranium and strontium isotope tracers of water sources and surface water-groundwater interactions in arid wetlands: Pahranagat Valley, Nevada, USA

    USGS Publications Warehouse

    Paces, James B.; Wurster, Frederic C.

    2014-01-01

    Near-surface physical and chemical process can strongly affect dissolved-ion concentrations and stable isotope compositions of water in wetland settings, especially under arid climate conditions. In contrast, heavy radiogenic isotopes of strontium (87Sr/86Sr) and uranium (234U/238U) remain largely unaffected and can be used to help identify unique signatures from different sources and quantify end-member mixing that would otherwise be difficult to determine. The utility of combined Sr and U isotopes are demonstrated in this study of wetland habitats on the Pahranagat National Wildlife Refuge, which depend on supply from large-volume springs north of the Refuge, and from small-volume springs and seeps within the Refuge. Water budgets from these sources have not been quantified previously. Evaporation, transpiration, seasonally variable surface flow, and water management practices complicate the use of conventional methods for determining source contributions and mixing relations. In contrast, 87Sr/86Sr and 234U/238U remain unfractionated under these conditions, and compositions at a given site remain constant. Differences in Sr- and U-isotopic signatures between individual sites can be related by simple two- or three-component mixing models. Results indicate that surface flow constituting the Refuge’s irrigation source consists of a 65:25:10 mixture of water from two distinct regionally sourced carbonate aquifer springs, and groundwater from locally sourced volcanic aquifers. Within the Refuge, contributions from the irrigation source and local groundwater are readily determined and depend on proximity to those sources as well as water management practices.

  5. A World without Sample Preparation: Developing Rapid Uranium Isotope Measurement Capabilities by Resonance Ionization Mass Spectrometry (RIMS)

    SciTech Connect

    Knight, K B; Hutcheon, I D; Isselhardt, B H; Savina, M R; Prussin, S G

    2009-06-08

    We are developing highly sensitive, highly discriminating laser-based techniques for rapid determination of isotopic compositions. Rapid command of such information is critical to assessment of the origin and history of nuclear materials, particularly in post-detonation scenarios.

  6. Regolith production rates calculated with Uranium-series isotopes at Shale Hills Critical Zone Observatory: implications on chemical weathering and landscape evolution

    NASA Astrophysics Data System (ADS)

    Ma, L.; Chabaux, F. J.; Pelt, E.; Blaes, E.; Jin, L.; Brantley, S. L.

    2009-12-01

    It is essential to understand the rates and mechanisms of regolith formation as it contributes to important Critical Zone processes such as nutrient cycling, carbon sequestration, erosion, and acid rain mitigation. Over the long term, the rates of weathering and erosion also combine to control the evolution of landscapes. Uranium-series isotopes offer a powerful tool to investigate regolith production rates and residence times within a weathering system because of their well-documented fractionation behavior during chemical weathering and transport by water. Here, we present a study of U-series isotopes (238U, 234U and 230Th) in soils developed on shale bedrock at the Shale Hills catchment in central Pennsylvania. (234U/238U) and (230Th/238U) activity ratios in samples collected from soil profiles along a planar hillslope in the catchment range from 0.934 to 1.072 and from 0.920 to 1.096, respectively. These values show significant U-series disequilibrium and are explained by a dual process of U-series isotopes during weathering: a loss of 234U, 238U, and 230Th during water-rock interactions and a gain of 234U and 238U as U precipitated from circulating soil water. Regolith production rates calculated with U-series isotopes for these soil profiles range from ~15 to 45 m/Myr and decrease systematically with increasing distance from the ridge top to the middle slope and to the valley floor. Soil residence times within these profiles increase from the ridge to the valley floor. The regolith production rates at Shale Hills vary as an exponential function of soil thickness, similar to the soil production functions derived from many other studies. With the local soil production function at Shale Hills, a hillslope soil transport model is used to predict the landscape evolution and change of soil thickness along the planar transect. The simulation results suggest that both the landscape and soil thickness along the planar hillscope at Shale Hills are currently at a

  7. The chemical and isotopic record of rock-water interaction in the Sherman Granite, Wyoming and Colorado

    NASA Astrophysics Data System (ADS)

    Zielinski, R. A.; Peterman, Z. E.; Stuckless, J. S.; Rosholt, J. N.; Nkomo, I. T.

    1982-01-01

    Chemical, isotopic, radiographic, and rock-leaching data are combined to describe the effects of rock-water interactions in core samples of petrographically fresh, 1.43 b.y.-old Sherman Granite. The data serve to identify sensitive indicators of incipient alteration and to estimate the degree, pathways, and timing of element mobilization. Unfractured core samples of Sherman Granite are remarkably fresh by most chemical or isotopic criteria, but incipient alteration is indicated by the abundance and distribution of uranium and the degree of radioactive equilibration of uranium with its decay products. Uranium abundances which are out of equilibrium with lead decay products indicate remobilization of a portion (3 to 60 percent) of original uranium in late Phanerozoic time. Association of uranium with minor but pervasive secondary alteration products also indicates some remobilization. The amount of apparent uranium mobility in unfractured Sherman Granite (3 to 60 percent) is small compared to the results of similar studies of Archean granites from nearby localities. Chemical and isotopic data evaluated as a function of core-sample depth suggest a uranium migrational pathway involving near-surface leaching and reconcentration at depth. Movement of solutions through the upper 200 ft (60 m) of Sherman Granite is fracture controlled, and brecciated granite shows more obvious petrographic, chemical, and isotopic evidence of alteration and multi-element redistribution. Laboratory experiments using freshly crushed Sherman Granite confirm that uranium is leached in preference to elements such as Si, Mg, Ca, and K, and that leachable uranium is situated close to the solid-liquid interface; perhaps as uranium along grain boundaries, in crystal defects, or on cleavage traces of minerals that exclude uranium from their structure.

  8. Uranium series and beryllium isotope evidence for an extended history of subduction modification of the mantle below Nicaragua

    SciTech Connect

    Reagan, M.K.; Herrstrom, E.A. ); Morris, J.D. ); Murrell, M.T. )

    1994-10-01

    U-series nuclides and beryllium and lead isotopes have been measured on historic lavas from eight volcanoes in Nicaragua. Low-Ti samples from northern Nicaragua have ([sup 230]Th)/([sup 232]Th) ratios from 2.23 to 2.56 and are enriched in [sup 238]U and [sup 234]U over [sup 230]Th by 1-16%. Those from southern Nicaragua have ([sup 230]Th)/([sup 232]Th) [approx] 2.1 and have ([sup 238]U)/([sup 230]Th) = 1.0-0.9. High-Ti samples have intermediate ([sup 230]Th)/([sup 232]Th) ratios and are strongly enriched in [sup 230]Th. Lead isotopic data for all samples plot in the mantle array with [sup 206]Pb/[sup 204]Pb = 18.50-18.63. Th isotopic ratios for all samples imply source U/Th ratios that are significantly higher than those implied by lead isotopic ratios. All historic samples have ([sup 210]Po)/([sup 230]Th) and thus ([sup 226]Ra)/([sup 230]Th) > 1, suggesting that lavas erupt less than 8,000 y after generation. Thorium isotopic ratios for all volcanic samples correlate well with [sup 10]Be/[sup 9]Be and B/Be as well as with [sup 87]Sr/[sup 86]Sr and Ba/La ratios from the literature. ([sup 238]U)/([sup 230]Th) ratios do not correlate well with any of these ratios but rather anti-correlate with Th concentrations and published La/Yb ratios. These observations, and inferences therefrom, lead to the following preferred, although not completely unique, interpretations. Comparison of thorium, beryllium, and strontium isotopic ratios of the Cocos plate sediments at DSDP 495 with the low-Ti volcanic regression trends shows that the subducted component transferred to the mantle has isotopic compositions similar to the bulk sediments. B/Be and Ba/La ratios of the volcanic samples are well correlated with the isotopes, but the inferred ratios in the subduction component are at least 10 and 5 times higher, respectively, than values in the bulk sediment.

  9. METHOD FOR PURIFYING URANIUM

    DOEpatents

    Kennedy, J.W.; Segre, E.G.

    1958-08-26

    A method is presented for obtaining a compound of uranium in an extremely pure state and in such a condition that it can be used in determinations of the isotopic composition of uranium. Uranium deposited in calutron receivers is removed therefrom by washing with cold nitric acid and the resulting solution, coataining uranium and trace amounts of various impurities, such as Fe, Ag, Zn, Pb, and Ni, is then subjected to various analytical manipulations to obtain an impurity-free uranium containing solution. This solution is then evaporated on a platinum disk and the residue is ignited converting it to U2/sub 3//sub 8/. The platinum disk having such a thin film of pure U/sub 2/O/sub 8/ is suitable for use with isotopic determination techaiques.

  10. Rapid determination of 226Ra and uranium isotopes in solid samples by fusion with lithium metaborate and alpha spectrometry.

    PubMed

    Bojanowski, R; Radecki, Z; Piekoś, R

    2002-07-01

    A simple and rapid method has been developed to determine 226Ra in rocks, soils, and sediments. Samples are decomposed by fusion with lithium metaborate and the melt is dissolved in a solution containing sulfates and citric acid. During the dissolution, a fine suspension of mixed barium and radium sulfates is formed. The microcrystals are collected on a membrane filter (pore size 0.1 microm) and analysed in an alpha spectrometer. Application of a 133Ba tracer enables us to assess the loss of the analyte, which only rarely exceeds 10%. All analytical operations, beginning from sample decomposition to source preparation for alpha spectrometry, can be accomplished within 1 or 2 h. With uranium determination, the filtrate is spiked with a 232U tracer and passed through a column loaded with a Dowex AG (1 x 4) anion-exchange resin in the sulfate form. Interfering elements are eluted with dilute sulfuric acid followed by concentrated hydrochloric acid. Uranium is eluted with water, electrodeposited on silver discs, and analysed in the alpha spectrometer. The method was tested on reference soil and sediment materials and was found to be accurate within the estimated uncertainties. PMID:12920318

  11. Environmental site description for a Uranium Atomic Vapor Laser Isotope Separation (U-AVLIS) production plant at the Oak Ridge Gaseous Diffusion Plant Site

    SciTech Connect

    Not Available

    1991-09-01

    In January 1990, the Secretary of Energy approved a plan for the demonstration and deployment of the Uranium Atomic Vapor Laser Isotope Separation (U-AVLIS) technology, with the near-term goal to provide the necessary information to make a deployment decision by November 1992. The U-AVLIS process is based on electrostatic extraction of photoionized U-235 atoms from an atomic vapor stream created by electron-beam vaporization of uranium metal alloy. A programmatic document for use in screening DOE sites to locate the U-AVLIS production plant was developed and implemented in two parts (Wolsko et al. 1991). The first part consisted of a series of screening analyses, based on exclusionary and other criteria, that identified a reasonable number of candidate sites. These sites were then subjected to a more rigorous and detailed comparative analysis for the purpose of developing a short list of reasonable alternative sites for later environmental examination. This environmental site description (ESD) provides a detailed description of the ORGDP site and vicinity suitable for use in an environmental impact statement (EIS). The report is based on existing literature, data collected at the site, and information collected by Argonne National Laboratory (ANL) staff during a site visit. The organization of the ESD is as follows. Topics addressed in Sec. 2 include a general site description and the disciplines of geology, water resources, biotic resources, air resources, noise, cultural resources, land use, socioeconomics, and waste management. Identification of any additional data that would be required for an EIS is presented in Sec. 3. Following the site description and additional data requirements, Sec. 4 provides a short, qualitative assessment of potential environmental issues. 37 refs., 20 figs., 18 tabs.

  12. Uranium thorium chronometry of weathering rinds: Rock alteration rate and paleo-isotopic record of weathering fluids

    NASA Astrophysics Data System (ADS)

    Pelt, E.; Chabaux, F.; Innocent, C.; Navarre-Sitchler, A. K.; Sak, P. B.; Brantley, S. L.

    2008-11-01

    The potential of 238U- 234U- 230Th chronometry for constraining the formation rate of weathering rinds developed on fresh rocks is assessed by analyzing a weathering rind on a basaltic clast from a 125 kyr old Costa Rican alluvial terrace. Eighteen subsamples were collected from one section of the clast by drilling cores (4 mm in diameter and 5 mm depth) along two transects straddling the core-rind boundary. Variations of major and trace element concentrations along the two transects point out (a) intense loss of alkaline and alkaline-earth elements, (b) conservative behaviour of elements such as Zr, Hf and Th, and (c) external input of U into the rind without any evidence of U loss during basalt weathering. In addition, variations in U concentrations along the transects show that the main U-Th fractionation process associated with the weathering of the basaltic clast is an external input of U (without addition nor loss of Th) in the basalt rind transition zone, and that, once deposited U is immobile in the weathering rind. In the frame of this interpretation scheme, a weathering rate of 0.5 ± 0.2 mm/kyr can be calculated for the studied clast, which is consistent with geological and isotopic evidence constraining the depositional ages of the terraces. In addition, the variations in the ( 234U/ 238U) ratio along the analysed transects as well as the increase in Sr isotopic ratios within the weathering rind are best explained by temporal variation of the U activity ratios and Sr isotope ratios of the soil solutions brought into the rind. This work highlights how well detailed U-Th chronological studies of weathering rinds can (1) constrain the formation rates of weathering systems, and (2) record the time variation of isotopic composition of weathering fluids.

  13. Micro-analytical uranium isotope and chemical investigations of zircon crystals from the Chernobyl "lava" and their nuclear fuel inclusions

    NASA Astrophysics Data System (ADS)

    Pöml, P.; Burakov, B.; Geisler, T.; Walker, C. T.; Grange, M. L.; Nemchin, A. A.; Berndt, J.; Fonseca, R. O. C.; Bottomley, P. D. W.; Hasnaoui, R.

    2013-08-01

    U isotope data measured on real fragments of the Chernobyl nuclear fuel included in zircon crystals crystallised from the Chernobyl "lava" are presented for the first time. The U isotope data show no anomalies and lie within the expected burnup values for the Chernobyl nuclear fuel. However, the U concentration, the U isotopic composition, and the Ti concentration in the host zircon vary significantly within single crystals as well as between single crystals. Our results indicate that during the time of melt activity temperature and melt composition likely varied considerably. New melt was formed progressively (and solidified) during the accident that reacted and mixed with pre-existing melt that never fully equilibrated. In such an environment zircon crystals crystallised at temperatures below 1250 °C, as estimated from thermodynamic considerations along with the observation that the centre of the investigated zircon crystal contains monoclinic ZrO2 inclusions. Since the zircon crystals crystallised before the silicate melt spread out into the reactor block basement, the flow of the melt into the basement must also have occurred at temperatures below 1250 °C.

  14. Nuclear forensic analysis of uranium oxide powders interdicted in Victoria, Australia

    DOE PAGESBeta

    Kristo, Michael Joseph; Keegan, Elizabeth; Colella, Michael; Williams, Ross; Lindvall, Rachel; Eppich, Gary; Roberts, Sarah; Borg, Lars; Gaffney, Amy; Plaue, Jonathan; et al

    2015-04-13

    Nuclear forensic analysis was conducted on two uranium samples confiscated during a police investigation in Victoria, Australia. The first sample, designated NSR-F-270409-1, was a depleted uranium powder of moderate purity (~1000 μg/g total elemental impurities). The chemical form of the uranium was a compound similar to K2(UO2)3O4·4H2O. While aliquoting NSR-F-270409-1 for analysis, the body and head of a Tineid moth was discovered in the sample. The second sample, designated NSR-F-270409-2, was also a depleted uranium powder. It was of reasonably high purity (~380 μg/g total elemental impurities). The chemical form of the uranium was primarily UO3·2H2O, with minor phases ofmore » U3O8 and UO2. While aliquoting NSR-F-270409-2 for analysis, a metal staple of unknown origin was discovered in the sample. The presence of 236U and 232U in both samples indicates that the uranium feed stocks for these samples experienced a neutron flux at some point in their history. The reactor burn-up calculated from the isotopic composition of the uranium is consistent with that of spent fuel from natural uranium (NU) fueled Pu production. These nuclear forensic conclusions allow us to categorically exclude Australia as the origin of the material and greatly reduce the number of candidate sources.« less

  15. Uranium and molybdenum isotope evidence for an episode of widespread ocean oxygenation during the late Ediacaran Period

    NASA Astrophysics Data System (ADS)

    Kendall, Brian; Komiya, Tsuyoshi; Lyons, Timothy W.; Bates, Steve M.; Gordon, Gwyneth W.; Romaniello, Stephen J.; Jiang, Ganqing; Creaser, Robert A.; Xiao, Shuhai; McFadden, Kathleen; Sawaki, Yusuke; Tahata, Miyuki; Shu, Degan; Han, Jian; Li, Yong; Chu, Xuelei; Anbar, Ariel D.

    2015-05-01

    To improve estimates of the extent of ocean oxygenation during the late Ediacaran Period, we measured the U and Mo isotope compositions of euxinic (anoxic and sulfidic) organic-rich mudrocks (ORM) of Member IV, upper Doushantuo Formation, South China. The average δ238U of most samples is 0.24 ± 0.16‰ (2SD; relative to standard CRM145), which is slightly higher than the average δ238U of 0.02 ± 0.12‰ for restricted Black Sea (deep-water Unit I) euxinic sediments and is similar to a modeled δ238U value of 0.2‰ for open ocean euxinic sediments in the modern well-oxygenated oceans. Because 238U is preferentially removed to euxinic sediments compared to 235U, expanded ocean anoxia will deplete seawater of 238U relative to 235U, ultimately leading to deposition of ORM with low δ238U. Hence, the high δ238U of Member IV ORM points to a common occurrence of extensive ocean oxygenation ca. 560 to 551 Myr ago. The Mo isotope composition of sediments deposited from strongly euxinic bottom waters ([H2S]aq >11 μM) either directly records the global seawater Mo isotope composition (if Mo removal from deep waters is quantitative) or represents a minimum value for seawater (if Mo removal is not quantitative). Near the top of Member IV, δ98Mo approaches the modern seawater value of 2.34 ± 0.10‰. High δ98Mo points to widespread ocean oxygenation because the preferential removal of isotopically light Mo to sediments occurs to a greater extent in O2-rich compared to O2-deficient marine environments. However, the δ98Mo value for most Member IV ORM is near 0‰ (relative to standard NIST SRM 3134 = 0.25‰), suggesting extensive anoxia. The low δ98Mo is at odds with the high Mo concentrations of Member IV ORM, which suggest a large seawater Mo inventory in well-oxygenated oceans, and the high δ238U. Hence, we propose that the low δ98Mo of most Member IV ORM was fractionated from contemporaneous seawater. Possible mechanisms driving this isotope fractionation include

  16. Predicted discharge plutonium isotopics for LEU [low-enriched uranium] test pebble irradiated in the AVR [Arbeitsgemeinschaft Versuchsreaktor

    SciTech Connect

    Lane, R.K.; Lefler, W.L.

    1988-06-01

    A Subprogram Plan related to the Arbeitsgemeinschaft Versuchsreaktor (AVR) Test Program is in place and describes cooperative work being carried out under the United States/Federal Republic of Germany (US/FRG) Implementing Agreement for Cooperation in Gas-Cooled Reactor Development. The AVR information to be provided as described in the plan will provide a basis for examining the accuracy of computational methods used for performance and safety analysis. The purpose of the cooperation is to obtain experimental information from the AVR relevant to the performance and safety of modular gas-cooled reactors, and to compare measured results with predictions of analytical tools. This report provides a progress report on the prediction of plutonium buildup in LEU fuel in a high-enriched uranium (HEU) core and also describes the method for calculating the U-238 resonance integral (cross section). 4 refs., 5 figs., 11 tabs.

  17. Quantifying regolith production rates with Uranium-series isotopes at Shale Hills Critical Zone Observatory: implications for chemical weathering and landscape evolution

    NASA Astrophysics Data System (ADS)

    Ma, Lin; Chabaux, Francois; Pelt, Eric; Blaes, Estelle; Jin, Lixin; Brantley, Susan

    2010-05-01

    Quantifying regolith production rates is essential in understanding many important Earth's surface processes such as nutrient cycling, carbon sequestration, erosion, and acid rain mitigation. Over the long term, the rates of weathering and erosion also combine to control the evolution of surface landscapes. Uranium-series isotopes offer a powerful tool to investigate regolith production rates and weathering timescales within a weathering system because of their well-documented fractionation behavior during chemical weathering and transport by water. To quantify regolith formation rates on shale lithology, we measured U-series isotopes (238U, 234U, and 230Th) in three weathering soil profiles along a planar north-facing hillslope at the Susquehanna Shale Hills Observatory (SSHO) in central Pennsylvania. All regolith samples show significant U-series disequilibrium: (234U/238U) and (230Th/238U) activity ratios range from 0.934 to 1.072 and from 0.903 to 1.096, respectively. These values display depth trends that are consistent with fractionation of U-series isotopes during chemical weathering, i.e., the relative mobility decreases in the order 234U > 238U >> 230Th. The activity ratios observed in the soils are explained by i) loss of U-series isotopes during water-rock interactions and ii) re-precipitation of 234U and 238U downslope. Regolith production rates calculated with U-series isotopes for these soil profiles decrease systematically with increasing distance from the ridge: from ~45 m/Myr at the ridge top, the highest point along the hillslope, to ~26 m/Myr at the middle slope site, and to ~15 m/Myr at the valley floor. Soil weathering timescales within these profiles range from 7 kyr to 45 kyr, increasing from the ridge to the valley floor. Given that the SSHO experienced peri-glacial climate ~15 ky ago, we conclude that the hillslope retains regolith formed before that glacial period and that the hillslope is not at geomorphological steady state. The regolith

  18. A review of applications of U-Th-Pb isotope systematics to investigations of uranium source rocks.

    USGS Publications Warehouse

    Stuckless, J.S.

    1987-01-01

    U, Th and Pb concentrations and the isotopic composition of Pb can be used to evaluate crystalline rocks as a source for U in sedimentary deposits. Under favourable geologic circumstances, the technique can yield information on both the timing and the amount of U released to the sedimentary environment. The technique is best suited to the study of Archean rocks that have high U/Pb, a known common Pb composition, and a simple two-stage history. Less ideal rock units can also be evaluated, but conclusions reached for rocks of Phanerozoic age or younger will generally be qualitative at best.-Author

  19. Uranium-lead Isotope Evidence in the Shelyabinsk LL5 Chondrite Meteorite for Ancient and Recent Thermal Events

    NASA Technical Reports Server (NTRS)

    Lapen, T. J.; Kring, D. A.; Zolensky, M. E.; Andreasen, R.; Righter, M.; Swindle, T. D.; Beard, S. P.; Swindle, T. D.

    2014-01-01

    The impact histories on chondrite parent bodies can be deduced from thermochronologic analyses of materials and isotope systems with distinct apparent closure temperatures. It is especially critical to better understand the geological histories and physical properties of potenally hazardous near-Earth asteroids. Chelyabinsk is an LL5 chondrite meteorite that was dispersed over a wide area tens of kilometers south of the town of Chelyabinsk, Russia by an explosion at an altitude of 27 km at 3:22 UT on 15 Feb 2013 [1,2]. The explosion resulted in significant damage to surrounding areas and over 1500 injuries along with meteorite fragments being spread over a wide area [1].

  20. Uranium-Lead Zircon Ages and Sr, Nd, and Pb Isotope Geochemistry of Selected Plutonic Rocks from Western Idaho

    USGS Publications Warehouse

    Unruh, Daniel M.; Lund, Karen; Kuntz, Mel A.; Snee, Lawrence W.

    2008-01-01

    Across the Salmon River suture in western Idaho, where allochthonous Permian to Cretaceous oceanic rocks are juxtaposed against Proterozoic North American rocks, a wide variety of plutonic rocks are exposed. Available data indicate much variation in composition, source, and structural state of these plutons. The plutonic rocks were long described as the western border zone of the Cretaceous Idaho batholith but limited pre-existing age data indicate more complicated origins. Because the affinity and age of the plutonic rocks cannot be reliably determined from field relations, TIMS U-Pb dating in conjunction with Sr, Nd, and Pb isotopic studies of selected plutons across the suture in western Idaho were undertaken. The data indicate three general groups of plutons including (1) those that intruded the island arc terranes during the Triassic and Jurassic, those that intruded near the western edge of oceanic rocks along the suture in the Early Cretaceous, and the plutons of the Idaho batholith that intruded Proterozoic North American rocks in the Late Cretaceous. Plutons that intruded Proterozoic North American rocks commonly include xenocrystic zircons and in several cases, ages could not be determined. The least radiogenic Sr and most radiogenic Nd are found among the Blue Mountains superterrane island arc samples. Suture-zone plutons have isotopic characteristics that span the range between Idaho batholith and island arc samples but mostly follow island arc signatures. Plutons of the Idaho batholith have the most radiogenic initial Pb and Sr ratios and the least radiogenic Nd of the samples analyzed.

  1. Uranium and Strontium Isotopic Study of the Hydrology of the Alluvial Aquifer at the Rifle Former U Mine Tailings Site, Colorado

    NASA Astrophysics Data System (ADS)

    Christensen, J. N.; Shiel, A. E.; Conrad, M. E.; Williams, K. H.; Dong, W.; Tokunaga, T. K.; Wan, J.; Long, P. E.; Hubbard, S. S.

    2014-12-01

    The Rifle Site consists of a floodplain along the Colorado River that was remediated through the removal of surface material underlying former uranium-vanadium mill tailings. The semi-arid (precip. = ~30 cm/year) catchment for the site has an area of ~1km2. The Rifle Site provides an excellent field laboratory for the study of the fluxes of water and carbon from the vadose zone to groundwater (LBNL SFA2.0, http://esd.lbl.gov/research/projects/sssfa2/). A network of monitoring wells, particularly a set instrumented in the vadose zone, provide the opportunity to closely sample groundwater and vadose zone porewater both in space and time. In order to better understand the spatial and temporal variation of vadose zone interaction with groundwater within the Rifle floodplain and provide constraints for a Rifle hydrological model, we have analyzed the Sr isotopic compositions, 234U/238U activity ratios, and d238U of groundwater, vadose zone porewater (sampled through depth-distributed lysimeters) and surface water including the Colorado River. Significant contrasts in 87Sr/86Sr and 234U/238U allow the identification of different sources contributing to Rifle groundwater, while d238U provides an additional tracer and insights into redox processes. Vadose zone porewater is characterized by high 87Sr/86Sr and Sr concentrations and falls at one end of a mixing line with Rifle groundwater, while upgradient groundwater with lower 87Sr/86Sr and Sr concentrations falls at the other end. A mixing model using vadose zone porewater and upgradient groundwater as endmembers suggests that the contribution of vertical recharge through the floodplain increases to ~20% systematically across the floodplain towards the Colorado River. An exception to this pattern is a well located 150m from the river with recent high U concentrations (>300 ppb) and U and Sr isotopic compositions consistent with a 38% vadose zone contribution. U and Sr isotopes show that an irrigation-return ditch that cuts

  2. RECOVERY OF URANIUM FROM PITCHBLENDE

    DOEpatents

    Ruehle, A.E.

    1958-06-24

    The decontamination of uranium from molybdenum is described. When acid solutions containing uranyl nitrate are contacted with ether for the purpose of extracting the uranium values, complex molybdenum compounds are coextracted with the uranium and also again back-extracted from the ether with the uranium. This invention provides a process for extracting uranium in which coextraction of molybdenum is avoided. It has been found that polyhydric alcohols form complexes with molybdenum which are preferentially water-soluble are taken up by the ether extractant to only a very minor degree. The preferred embodiment of the process uses mannitol, sorbitol or a mixture of the two as the complexing agent.

  3. Coupling of Uranium and Thorium Series Isotope Systematics for Age Determination of Late Pleistocene Zircons using LA-ICP-MS

    NASA Astrophysics Data System (ADS)

    Sakata, S.; Hirakawa, S.; Iwano, H.; Danhara, T.; Hirata, T.

    2014-12-01

    Zircon U-Th-Pb dating method is one of the most important tools for estimating the duration of magmatism by means of coupling of uranium, actinium and thorium decay series. Using U-Pb dating method, its reliability is principally guaranteed by the concordance between 238U-206Pb and 235U-207Pb ages. In case of dating Quaternary zircons, however, the initial disequilibrium effect on 230Th and 231Pa should be considered. On the other hands, 232Th-208Pb dating method can be a simple but powerful approach for investigating the age of crystallization because of negligible influence from initial disequilibrium effect. We have developed a new correction model for accurate U-Pb dating of the young zircon samples by taking into consideration of initial disequilibrium and a U-Pb vs Th-Pb concordia diagram for reliable age calibration was successfully established. Hence, the U-Th-Pb dating method can be applied to various zircons ranging from Hadean (4,600 Ma) to Quaternary (~50 ka) ages, and this suggests that further detailed information concerning the thermal history of the geological sequences can be made by the coupling of U-Th-Pb, fission track and Ar-Ar ages. In this presentation, we will show an example of U-Th-Pb dating for zircon samples from Sambe Volcano (3 to 100 ka), southwest Japan and the present dating technique using LA-ICP-MS.

  4. The Sahara-East Mediterranean dust and climate connection revealed by strontium and uranium isotopes in a Jerusalem speleothem

    NASA Astrophysics Data System (ADS)

    Frumkin, Amos; Stein, Mordechai

    2004-01-01

    This paper explores the potential of Sr and U isotope systems in speleothems as tracers of eolian dust transport and hydrological conditions. The study focuses on a speleothem from Jerusalem spanning the past 220 kyr. This speleothem provides a precisely dated record of dust flux from the Sahara to the East Mediterranean. Enhanced dust flux and Terra Rossa soil development are reflected by elevated 87Sr/ 86Sr ratios in the speleothem (0.7082-0.7086), while lower 87Sr/ 86Sr ratios (˜0.7078) indicate higher contribution of the local bedrock due to low dust flux and low soil accumulation. The strontium isotope system in the speleothem is a robust monitor of the Sahara monsoon-modulated climate, since dust uptake is related to development or reduction in vegetation cover of Sahara soil. The [ 234U/ 238U] activity ratios in the speleothem range between 1.12 and 1.0. The high activity values may indicate selective removal of 234U from the soil while the low values converge to the bedrock. The migration of 234U to the cave reflects mainly the regional hydrological conditions that are modulated by the North Atlantic-Mediterranean climate system. Thus, the speleothem provides a combined record of the monsoon-North Atlantic climatic systems. Long-term stability in glacial 87Sr/ 86Sr ratios (0.7083±0.0001 over the past 220 kyr) suggests an overall similarity in eolian dust sources, and uniformity in the synoptic conditions that dominate the dust storm tracks during glacial periods.

  5. High resolution analysis of uranium and thorium concentration as well as U-series isotope distributions in a Neanderthal tooth from Payre (Ardèche, France) using laser ablation ICP-MS

    NASA Astrophysics Data System (ADS)

    Grün, Rainer; Aubert, Maxime; Joannes-Boyau, Renaud; Moncel, Marie-Hélène

    2008-11-01

    We have mapped U ( 238U) and Th ( 232Th) elemental concentrations as well as U-series isotope distributions in a Neanderthal tooth from the Middle Palaeolithic site of Payre using laser ablation ICP-MS. The U-concentrations in an enamel section varied between 1 and 1500 ppb. The U-concentration maps show that U-migration through the external enamel surface is minute, the bulk of the uranium having migrated internally via the dentine into the enamel. The uranium migration and uptake is critically dependent on the mineralogical structure of the enamel. Increased U-concentrations are observed along lineaments, some of which are associated with cracks, and others may be related to intra-prismatic zones or structural weaknesses reaching from the dentine into the enamel. The uranium concentrations in the dentine vary between about 25,000 and 45,000 ppb. Our systematic mapping of U-concentration and U-series isotopes provides insight into the time domain of U-accumulation. Most of the uranium was accumulated in an early stage of burial, with some much later overprints. None of the uranium concentration and U-series profiles across the root of the tooth complied with a single stage diffusion-adsorption (D-A) model that is used for quality control in U-series dating of bones and teeth. Nevertheless, in the domains that yielded the oldest apparent U-series age estimates, U-leaching could be excluded. This means that the oldest apparent U-series ages of around 200 ka represent a minimum age for this Neanderthal specimen. This is in good agreement with independent age assessments (200-230 ka) for the archaeological layer, in which it was found. The Th elemental concentrations in the dental tissues were generally low (between about 1 and 20 ppb), and show little relationship with the nature of the tissue.

  6. Using Uranium-Series Isotopes to Quantify Volcanic Soil Formation Rates Under a Tropical Climate: Basse-Terre, Guadeloupe

    NASA Astrophysics Data System (ADS)

    Pereyra, Y.; Ma, L.; Sak, P. B.; Gaillardet, J.; Buss, H. L.; Brantley, S. L.

    2014-12-01

    U-series isotopes fractionate during chemical weathering and their activity ratios have been used to determine timescales and rates of soil formation. Such soil formation rates are measured at soil profile scale and provide an important link to compare chemical weathering rates measured across different spatial scales. We analyzed U-series isotope compositions in a ~12m deep soil profile in Basse-Terre Island of French Guadeloupe. The tropical Bras David watershed is developed on andesitic pyroclastic flows. Field observations have shown heterogeneity in color and texture in this profile. However, major element chemistry and mineralogy show some general depth trends. First, Al, Fe, and Ti show a depletion profile relative to Th from 12m to 4m depth, an addition from 4m to 2m, and depletion from 2m to the surface. Second, mobile elements such as Ca, Mg, and Sr have undergone intensive weathering, therefore show almost complete depletion even in the deep profile, and an addition profile near the surface. This addition trend is most likely related to atmospheric dust and marine aerosol signatures. Finally, K, Mn, and Si show a partial depletion profile at depth. The main minerals present throughout the soil profile are halloysite and gibbsite. 238U/232Th ratios in this profile ranged from 0.374 to 1.696, while the 230Th/232Th ratios ranged from 0.367 to 1.701. A decrease of (238U/232Th) in the deep soil profile from 12m to 4m depth is observed, and an increase in the shallow profile from 4m to the surface. The (230Th /232Th) ratios showed a similar trend as (238U/232Th). Marine aerosols and atmospheric dust are responsible for the addition of U in shallow soils while intensive chemical weathering is responsible for the loss of U at depth. U-series chemical weathering model suggests that the weathering duration from 12m to 4m depth is about 250kyr, with a weathering advancing rate of ~30 m/Ma. The rate is also about one order of magnitude lower than the weathering rate

  7. Uranium thorium hydride nuclear fuel

    SciTech Connect

    Simnad, M.T.

    1985-01-15

    A nuclear fuel includes uranium dispersed within a thorium hydride matrix. The uranium may be in the form of particles including fissile and non-fissile isotopes. Various hydrogen to thorium ratios may be included in the matrix. The matrix with the fissile dispersion may be used as a complete fuel for a metal hydride reactor or may be combined with other fuels.

  8. Uranium isotope compositions of the basaltic angrite meteorites and the chronological implications for the early Solar System

    PubMed Central

    Brennecka, Gregory A.; Wadhwa, Meenakshi

    2012-01-01

    Events occurring within the first 10 million years of the Solar System’s approximately 4.5 billion-year history, such as formation of the first solids, accretion, and differentiation of protoplanetary bodies, have determined the evolutionary course of our Solar System and the planetary bodies within it. The application of high-resolution chronometers based on short-lived radionuclides is critical to our understanding of the temporal sequence of these critical events. However, to map the relative ages from such chronometers onto the absolute time scale, they must be “anchored” to absolute ages of appropriate meteoritic materials using the high-precision lead–lead (Pb–Pb) chronometer. Previously reported Pb–Pb dates of the basaltic angrite meteorites, some of which have been used extensively as time anchors, assumed a constant 238U/235U ratio (= 137.88). In this work, we report measurements of 238U/235U ratios in several angrites that are distinct from the previously assumed value, resulting in corrections to the Pb–Pb ages of ≥1 million years. There is no resolvable variation in the 238U/235U ratio among the angrite bulk samples or mineral separates, suggesting homogeneity in the U isotopic composition of the angrite parent body. Based on these measurements, we recalculated the Pb–Pb age for the commonly used anchor, the D’Orbigny angrite, to be 4563.37 ± 0.25 Ma. An adjustment to the Pb–Pb age of a time anchor (such as D’Orbigny) requires a corresponding correction to the “model ages” of all materials dated using that anchor and a short-lived chronometer. This, in turn, has consequences for accurately defining the absolute timeline of early Solar System events. PMID:22647606

  9. Minority Report

    ERIC Educational Resources Information Center

    Honawar, Vaishali

    2006-01-01

    Stephanie Kwader is a white minority at the Bowie State University, a 5,500-student historically black university. Students like her belong to a small but growing group: minority students on the campuses of the nation's 105 historically black colleges and universities. HBCUs, as they are referred in the field, offer competitive academics with…

  10. Considerations in the Application of Multiple Ion Counting for the Trace Analysis of Plutonium and Uranium Isotope Ratios Using Thermal Ionization and Inductively-Coupled Plasma Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Riciputi, L. R.

    2008-12-01

    The use of simultaneous multiple-ion counting for the analysis of small samples of plutonium and uranium has been investigated using three different instruments, the ThermoElectron Neptune inductively-coupled plasma mass spectrometer, the ThermoElectron Triton thermal ionization mass spectrometer, and the Isotopex Iso-T thermal ionization mass spectrometer. The Neptune and Triton instruments utilize identical multiple ion counter arrays, with ions impinging directly on the channeltron surface. The Isotopex instruments utilize a different style of channeltron detector. The most significant difference in the Isotopex detectors is the presence of a conversion dynode at the entrance to the channeltron. Results suggest that the performance of the ThermoElectron MIC system varies between the Neptune and Triton instruments, which probably reflects both differences in the inherent characteristics of plasma and thermal sources and the performance of the MICS themselves. Differences in performance and stability between the '"naked"' and conversion dynode equipped channeltrons on the two thermal ionization instruments support these observations. These differences suggest that different analytical approaches to calibration of the multiple-ion counters may be required. Differences in potential analytical strategies employing multiple ion counters on the different instruments, including calibration schemes, precision and accuracy limits, and analytical strategies that can be employed, will be discussed. Results from both thermal ionization and inductively-coupled plasma sources suggest that the dominant source of uncertainty in isotope ratio measurement using multiple ion counting shifts from counting limitations for very small signals to uncertainties in gain calibration and detector drift among the ion counters at higher count rates. These characteristics place limits on the applicability of multiple ion counters; results from mixed Faraday/multiple ion counting analysis will

  11. Uranium: A Dentist's perspective

    PubMed Central

    Toor, R. S. S.; Brar, G. S.

    2012-01-01

    Uranium is a naturally occurring radionuclide found in granite and other mineral deposits. In its natural state, it consists of three isotopes (U-234, U-235 and U-238). On an average, 1% – 2% of ingested uranium is absorbed in the gastrointestinal tract in adults. The absorbed uranium rapidly enters the bloodstream and forms a diffusible ionic uranyl hydrogen carbonate complex (UO2HCO3+) which is in equilibrium with a nondiffusible uranyl albumin complex. In the skeleton, the uranyl ion replaces calcium in the hydroxyapatite complex of the bone crystal. Although in North India, there is a risk of radiological toxicity from orally ingested natural uranium, the principal health effects are chemical toxicity. The skeleton and kidney are the primary sites of uranium accumulation. Acute high dose of uranyl nitrate delays tooth eruption, and mandibular growth and development, probably due to its effect on target cells. Based on all previous research and recommendations, the role of a dentist is to educate the masses about the adverse effects of uranium on the overall as well as the dental health. The authors recommended that apart from the discontinuation of the addition of uranium to porcelain, the Public community water supplies must also comply with the Environmental Protection Agency (EPA) standards of uranium levels being not more than 30 ppb (parts per billion). PMID:24478959

  12. Using Uranium-series isotopes to understand processes of rapid soil formation in tropical volcanic settings: an example from Basse-Terre, French Guadeloupe

    NASA Astrophysics Data System (ADS)

    Ma, Lin

    2015-04-01

    Lin Ma1, Yvette Pereyra1, Peter B Sak2, Jerome Gaillardet3, Heather L Buss4 and Susan L Brantley5, (1) University of Texas at El Paso, El Paso, TX, United States, (2) Dickinson College, Carlisle, PA, United States, (3) Institute de Physique d Globe Paris, Paris, France, (4) University of Bristol, Bristol, United Kingdom, (5) Pennsylvania State University Main Campus, University Park, PA, United States Uranium-series isotopes fractionate during chemical weathering and their activity ratios can be used to determine timescales and rates of soil formation. Such soil formation rates provide important information to understand processes related to rapid soil formation in tropical volcanic settings, especially with respect to their fertility and erosion. Recent studies also highlighted the use of U-series isotopes to trace and quantify atmospheric inputs to surface soils. Such a process is particularly important in providing mineral nutrients to ecosystems in highly depleted soil systems such as the tropical soils. Here, we report U-series isotope compositions in thick soil profiles (>10 m) developed on andesitic pyroclastic flows in Basse-Terre Island of French Guadeloupe. Field observations have shown heterogeneity in color and texture in these thick profiles. However, major element chemistry and mineralogy show some general depth trends. The main minerals present throughout the soil profile are halloysite and gibbsite. Chemically immobile elements such as Al, Fe, and Ti show a depletion profile relative to Th while elements such as K, Mn, and Si show a partial depletion profile at depth. Mobile elements such as Ca, Mg, and Sr have undergone intensive weathering at depths, and an addition profile near the surface, most likely related to atmospheric inputs. (238U/232Th) activity ratios in one soil profile from the Brad David watershed in this study ranged from 0.374 to 1.696, while the (230Th/232Th) ratios ranged from 0.367 to 1.701. A decrease of (238U/232Th) in the

  13. Stable isotopes (δ 18O and δ 13C), trace and minor element compositions of Recent scleractinians and Last Glacial bivalves at the Santa Maria di Leuca deep-water coral province, Ionian Sea

    NASA Astrophysics Data System (ADS)

    Correa, Matthias López; Montagna, Paolo; Vendrell-Simón, Begoña; McCulloch, Malcolm; Taviani, Marco

    2010-03-01

    The aragonitic skeletons of bathyal cold-water corals have a high potential as geochemical in situ archives for paleoceanography. Oxygen isotopes and stable carbon isotopes (δ 18O and δ 13C) have been analyzed, as well as trace and minor element compositions (e.g. Mg/Ca, Sr/Ca, U/Ca, B/Ca and P/Ca) in Lophelia pertusa, one of the most important frame-builders at the Santa Maria di Leuca (SML) deep-water coral hotspot in the Central Mediterranean. The Apulian Bank is swept by strong currents of the Adriatic Deep Water Outflow. The temperature of 13.9 °C is the highest temperature recorded for L. pertusa and provides an important end-member of environmental conditions for geochemical analyses on living Atlantic and Mediterranean cold-water corals. Temperature and salinity (38.77 PSU) are stable throughout the year, and thus virtually no changes should be observed in the stable oxygen isotope signal—if the coral precipitates its skeleton in equilibrium with seawater. We measured various marine properties, such as the seawater oxygen isotope composition (δ 18O sw), stable carbon isotope composition (δ 13C DIC) of dissolved inorganic carbon (DIC), and dissolved inorganic nutrient concentrations (PO 4, NO 3, NO 2, NH 3 and SiO 2). Bottom water at the coral sites shows a mean oxygen isotope composition of 1.47‰ δ 18O sw-VSMOW, and δ 13C DIC showed a mean of 1.1‰ VPDB. A section of a living L. pertusa with a thick theca calcification was probed with a Merchantek MicroMill at a high spatial sampling resolution with 10 samples per 1 mm. This reduced the signal-smoothing inherent to conventional sampling. The δ 18O ag of coral aragonite ranges between -2.0‰ and +2.8‰ VPDB and the δ 13C ag ranges between -7.77‰ and +1.47‰ VPDB. The Gaussian data distribution for both parameters, including heavy equilibrium values, suggests the completeness of the captured isotopic variability. The strict linear correlation of δ 13C and δ 18O displays a strong 'kinetic

  14. LA-ICP-MS analyses of minor and trace elements and bulk Ge isotopes in zoned Ge-rich sphalerites from the Noailhac - Saint-Salvy deposit (France): Insights into incorporation mechanisms and ore deposition processes

    NASA Astrophysics Data System (ADS)

    Belissont, Rémi; Boiron, Marie-Christine; Luais, Béatrice; Cathelineau, Michel

    2014-02-01

    sphalerite varies from -2.07 ± 0.37‰ to +0.91 ± 0.16‰ (2σ SD) and positively correlates with bulk Ge content. This indicates considerable Ge isotopic fractionation within sphalerite during low-T hydrothermal deposition and zoning processes, associated with possible microscale open system fluid mixing. The trace element features in sphalerite from Saint-Salvy compared with those of other deposits confirm their use as discriminators among genetic types of ores (e.g., high In contents for magmatic-related deposits, and Ge for low-temperature deposits). The LA-ICP-MS technique is revealed to be a powerful tool to measure in situ trace and minor elements occurring as solid solutions in sphalerite. The 74Ge isotope is most relevant for Ge analysis using the LA-ICP-MS, as this isotope shows the lowest isobaric interferences. Principal component analysis (PCA) of LA-ICP-MS dataset revealed an antithetic distribution of element clusters in sphalerite: Cu and trace elements Ge, Sb, Ag, and As are enriched and positively correlated in sector zoning whereas Fe, Cd, In and Sn are enriched in dark brown rhythmic bands. This distribution implies crystallographic controls on the incorporation of trace elements. Regardless of the zoning type, all spots considered, notable coupled substitutions have been suggested from binary scatter plots: 2Zn2+ ↔ Cu+ + Sb3+ and 3Zn2+ ↔ Ge4+ + 2Ag+. Also, the data suggest the substitution 3Zn2+ ↔ In3+ + Sn3+ + □ although Sn oxidation state needs verification using appropriate methods (e.g., XAS, μ-XANES/EXAFS). Fe and Cd are mainly involved in direct Zn2+ ↔ (Fe2+, Cd2+) substitutions. Noticeably, in all spots, Cu content approaches the sum of all available tri- and tetravalent cations. In this way, Cu (occurring as Cu+) could provide charge-balance for the entire broad set of coupled substitution mechanisms responsible for incorporation of the whole range of trace elements in Saint-Salvy sphalerite, especially Ge, Ga and Sb. Germanium

  15. Quantifying rind formation and chemical weathering rates in weathering clasts with uranium-series isotopes: a case study from Basse-Terre Island, Guadeloupe

    NASA Astrophysics Data System (ADS)

    Ma, L.; Chabaux, F. J.; Pelt, E.; Granet, M.; Sak, P. B.; Gaillardet, J.; Lebedeva, M.; Brantley, S. L.

    2011-12-01

    Weathering of tropical volcanic islands is rapid because of the reactive nature of the volcanic rock and the hot humid climate. In the tropics, rock fragments in the regolith zone commonly form alteration rinds. Weathering rinds are excellent samples to understand key chemical weathering processes. To quantify rock weathering rates in a tropical climate and to understand the environmental factors that control these rates, we combined a novel U-series isotopic technique with chemical and electron microprobe analyses to study weathering rinds formed at Basse-Terre Island, Guadeloupe. U-series isotopes and element concentrations were analyzed in a basaltic/andesitic weathering rind collected from the Bras David watershed on Basse-Terre Island. From the clast, core and rind samples were obtained by drilling along two linear profiles. Elemental profiles reveal that elemental loss varies in the order of Ca, Na, Sr > K, Mg, Rb > Mn > Si > Ba > Al > Fe, and Ti =0 across the core-rind interface, consistent with relative reactivity of phases in the clast from plagioclase ≈ pyroxene ≈ glass matrix > apatite > ilmenite. Elemental profiles also reveal conservative behavior of Th and external addition of U into the rind during clast weathering. Measured (234U/238U) activity ratios of the rind samples (1.001 to 1.031) are mostly higher than the core samples (average at ~1.003). Measured (238U/232Th) and (230Th/232Th) activity ratios of the core and rind samples range from 0.973 to 1.817, and 0.971 to 1.375, respectively. Most importantly, both (238U/232Th) and (230Th/232Th) activity ratios increase systematically from the core into the weathering rind for the two profiles. The elemental profiles and electronic microprobe observations suggest that weathering reactions include dissolution of pyroxene, plagioclase, and glass matrix, and formation of Fe oxyhydroxides, gibbsite and minor kaolinite. The dissolution of plagioclase leads to significant porosity growth within the rind

  16. Minority scholarships

    NASA Astrophysics Data System (ADS)

    The American Geological Institute sponsors undergraduate and graduate geoscience scholarships for members of ethnic minority groups. U.S. citizens who are majoring in geology, geophysics, geochemistry, hydrology, meteorology, oceanography, planetary geology, or Earth science education, and who are Black, Hispanic or Native American are eligible. Undergraduate awards can be as large as $10,000 a year; graduate awards, $4000 a year. Application deadline is February 1, 1990. Contact AGI Minority Participation Program Scholarships, American Geological Institute, 4220 King Street, Alexandria, VA 22302-1507; tel. 703-379-2480.

  17. An investigation into heterogeneity in a single vein-type uranium ore deposit: Implications for nuclear forensics.

    PubMed

    Keatley, A C; Scott, T B; Davis, S; Jones, C P; Turner, P

    2015-12-01

    Minor element composition and rare earth element (REE) concentrations in nuclear materials are important as they are used within the field of nuclear forensics as an indicator of sample origin. However recent studies into uranium ores and uranium ore concentrates (UOCs) have shown significant elemental and isotopic heterogeneity from a single mine site such that some sites have shown higher variation within the mine site than that seen between multiple sites. The elemental composition of both uranium and gangue minerals within ore samples taken along a single mineral vein in South West England have been measured and reported here. The analysis of the samples was undertaken to determine the extent of the localised variation in key elements. Energy Dispersive X-ray spectroscopy (EDS) was used to analyse the gangue mineralogy and measure major element composition. Minor element composition and rare earth element (REE) concentrations were measured by Electron Probe Microanalysis (EPMA). The results confirm that a number of key elements, REE concentrations and patterns used for origin location do show significant variation within mine. Furthermore significant variation is also visible on a meter scale. In addition three separate uranium phases were identified within the vein which indicates multiple uranium mineralisation events. In light of these localised elemental variations it is recommended that representative sampling for an area is undertaken prior to establishing the REE pattern that may be used to identify the originating mine for an unknown ore sample and prior to investigating impact of ore processing on any arising REE patterns. PMID:26301831

  18. Genetic implications of minor-element and Sr-isotope geochemistry of alkaline rock complexes in the Wet Mountains area, Fremont and Custer counties, Colorado

    USGS Publications Warehouse

    Armbrustmacher, T.J.; Hedge, C.E.

    1982-01-01

    Concentrations of Rb, Sr, and REE (rare earth elements), and Sr-isotopic ratios in rocks of the Cambrian alkaline complexes in the Wet Mountains area, Colorado, show that rocks formed as end-products of a variety of magmas generated from different source materials. The complexes generally contain a bimodal suite of cumulus mafic-ultramafic rocks and younger leucocratic rocks that include nepheline syenite and hornblende-biotite syenite in the McClure Mountain Complex, nepheline syenite pegmatite in the Gem Park Complex, and quartz syenite in the complex at Democrat Creek. The nepheline syenite and hornblende-biotite syenite at McClure Mountain (535??5m.y.) are older than the syenitic rocks at Democrat Creek (511??8m.y.). REE concentrations indicate that the nepheline syenite at McClure Mountain cannot be derived from the hornblende-biotite syenite, which it intrudes, or from the associated mafic-ultramafic rocks. REE also indicate that mafic-ultramafic rocks at McClure Mountain have a source distinct from that of the mafic-ultramafic rocks at Democrat Creek. In the McClure Mountain Complex, initial87Sr/86Sr ratios for mafic-ultramafic rocks (0.7046??0.0002) are similar to those of hornblende-biotite syenite (0.7045??0.0002), suggesting a similar magmatic source, whereas ratios for carbonatites (0.7038??0.0002) are similar to those of nepheline syenite (0.7038??0.0002). At Democrat Creek, initial ratios of syenitic rocks (0.7032??0.0002) and mafic-ultramafic rocks (0.7028??0.0002) are different from those of corresponding rocks at McClure Mountain. ?? 1982 Springer-Verlag.

  19. Nuclear forensic analysis of uranium oxide powders interdicted in Victoria, Australia

    SciTech Connect

    Kristo, Michael Joseph; Keegan, Elizabeth; Colella, Michael; Williams, Ross; Lindvall, Rachel; Eppich, Gary; Roberts, Sarah; Borg, Lars; Gaffney, Amy; Plaue, Jonathan; Knight, Kim; Loi, Elaine; Hotchkis, Michael; Moody, Kenton; Singleton, Michael; Robel, Martin; Hutcheon, Ian

    2015-04-13

    Nuclear forensic analysis was conducted on two uranium samples confiscated during a police investigation in Victoria, Australia. The first sample, designated NSR-F-270409-1, was a depleted uranium powder of moderate purity (~1000 μg/g total elemental impurities). The chemical form of the uranium was a compound similar to K2(UO2)3O4·4H2O. While aliquoting NSR-F-270409-1 for analysis, the body and head of a Tineid moth was discovered in the sample. The second sample, designated NSR-F-270409-2, was also a depleted uranium powder. It was of reasonably high purity (~380 μg/g total elemental impurities). The chemical form of the uranium was primarily UO3·2H2O, with minor phases of U3O8 and UO2. While aliquoting NSR-F-270409-2 for analysis, a metal staple of unknown origin was discovered in the sample. The presence of 236U and 232U in both samples indicates that the uranium feed stocks for these samples experienced a neutron flux at some point in their history. The reactor burn-up calculated from the isotopic composition of the uranium is consistent with that of spent fuel from natural uranium (NU) fueled Pu production. These nuclear forensic conclusions allow us to categorically exclude Australia as the origin of the material and greatly reduce the number of candidate sources.

  20. TERNARY ALLOYS OF URANIUM, COLUMBIUM, AND ZIRCONIUM

    DOEpatents

    Foote, F.G.

    1960-08-01

    Ternary alloys of uranium are described which are useful as neutron- reflecting materials in a fast neutron reactor. They are especially resistant to corrosion caused by oxidative processes of gascous or aqueous origin and comprise uranium as the predominant metal with zirconiunn and niobium wherein the total content of the minor alloying elements is between 2 and 8% by weight.

  1. The origin of breccia-hosted uranium deposits in carbonaceous metasediments of the Iberian Peninsula: U-Pb geochronology and stable isotope studies of the Fe deposit, Salamanca Province, Spain

    SciTech Connect

    Both, R.A. . Dept. of Geology and Geophysics); Arribas, A. . Dept. de Ingenieria Geologica); Saint-Andre, B. de . Lab. de Geochimie Isotopique)

    1994-05-01

    The Upper Proterozoic-Lower Cambrian schist-graywacke complex of the Iberian peninsula hosts several important uranium deposits, which are characterized by their occurrence in fracture and breccia zones and by the mineral association pitchblende + coffinite + carbonates + adularia + Fe sulfides. The Fe mine, in Salamanca province, is not only the largest known deposit of this type but also the most important uranium deposit in Spain, with current reserves in excess of 16,000 metric tons of U[sub 3]O[sub 8]. Primary mineralization occurs as narrow veins occupying fractures and in cavities as finely laminated sediments showing a variety of geopetal textures. Three stages of primary mineralization, separated by episodes of fracturing and brecciation, are recognized. Chlorite compositions and fluid inclusion data show that wall-rock alteration and ore deposition took place over a temperature range of approximately 280[degree] to less than 60 C, probably to subsurficial temperatures in the final stage of mineralization. The combined geologic evidence suggests deposition of the ore from a hydrothermal system that formed in response to the effects of Alpine tectonics on the Variscan basement. Meteoric water descended via steeply dipping faults, and as well as undergoing extensive isotope exchange with, also leached uranium and other components from, the metasediments of the schist-graywacke complex, particularly carbonaceous slates. The fluid was probably expelled toward the surface through the fracture and breccia system by seismic pumping. The episodic nature of the mineralization may have been controlled by fault movements that initiated brecciation and release of fluid pressure, leading to ore deposition in fractures and cavities.

  2. Minority Fellowships

    NASA Astrophysics Data System (ADS)

    Carlowicz, Michael

    In an effort to increase the number of ethnic minorities on the faculties of American colleges and universities, the Ford Foundation is offering fellowships to members of six groups who have been severely underrepresented in academia.In a program administered by the National Research Council (NRC), the Ford Foundation is offering 50 three-year predoctoral fellowships ($14,000 per year, plus a $6000 annual institutional grant) and 25 one-year dissertation fellowships ($18,000 for one year) to Native American Indians, Alaskan natives (Eskimos, Aleuts), Black/African Americans, Mexican Americans/Chicanos, Native Pacific Islanders (Polynesians and Micronesians), and Puerto Ricans. Fellowships will be awarded in the behavioral and social sciences, humanities, engineering, mathematics, physical sciences, life sciences, or interdisciplinary programs composed of two or more of those disciplines. The predoctoral fellowships are intended for beginning graduate students; the dissertation fellowships are designed to provide support for students in their final year.

  3. URANIUM RECOVERY

    DOEpatents

    Fitch, F.T.; Cruikshank, A.J.

    1958-10-28

    A process for recovering uranium from a solution of a diethyl dithiocarbaruate of uranium in an orgakic solvent substantially immiscible with water is presented. The process comprises brlnging the organic solutlon into intimate contact wlth an aqueous solution of ammonium carbonate, whereby the uranium passes to the aqueous carbonate solution as a soluble uranyl carbonate.

  4. Dry phase reactor for generating medical isotopes

    DOEpatents

    Mackie, Thomas Rockwell; Heltemes, Thad Alexander

    2016-05-03

    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.

  5. Impacts of Dust on Tropical Volcanic Soil Formation: Insights from Strontium and Uranium-Series Isotopes in Soils from Basse-Terre Island, French Guadeloupe

    NASA Astrophysics Data System (ADS)

    Pereyra, Y.; Ma, L.; Sak, P. B.; Gaillardet, J.; Buss, H. L.; Brantley, S. L.

    2015-12-01

    Dust inputs play an important role in soil formation, especially for thick soils developed on tropical volcanic islands. In these regions, soils are highly depleted due to intensive chemical weathering, and mineral nutrients from dusts have been known to be important in sustaining soil fertility and productivity. Tropical volcanic soils are an ideal system to study the impacts of dust inputs on the ecosystem. Sr and U-series isotopes are excellent tracers to identify sources of materials in an open system if the end-members have distinctive isotope signatures. These two isotope systems are particularly useful to trace the origin of atmospheric inputs into soils and to determine rates and timescales of soil formation. This study analyzes major elemental concentrations, Sr and U-series isotope ratios in highly depleted soils in the tropical volcanic island of Basse-Terre in French Guadeloupe to determine atmospheric input sources and identify key soil formation processes. We focus on three soil profiles (8 to 12 m thick) from the Bras-David, Moustique Petit-Bourg, and Deshaies watersheds; and on the adjacent rivers to these sites. Results have shown a significant depletion of U, Sr, and major elements in the deep profile (12 to 4 m) attributed to rapid chemical weathering. The top soil profiles (4 m to the surface) all show addition of elements such as Ca, Mg, U, and Sr due to atmospheric dust. More importantly, the topsoil profiles have distinct Sr and U-series isotope compositions from the deep soils. Sr and U-series isotope ratios of the top soils and sequential extraction fractions confirm that the sources of the dust are from the Saharan dessert, through long distance transport from Africa to the Caribbean region across the Atlantic Ocean. During the transport, some dust isotope signatures may also have been modified by local volcanic ashes and marine aerosols. Our study highlights that dusts and marine aerosols play important roles in element cycles and

  6. Evidence from molybdenum and iron isotopes and molybdenum-uranium covariation for sulphidic bottom waters during Eastern Mediterranean sapropel S1 formation

    NASA Astrophysics Data System (ADS)

    Azrieli-Tal, I.; Matthews, A.; Bar-Matthews, M.; Almogi-Labin, A.; Vance, D.; Archer, C.; Teutsch, N.

    2014-05-01

    Redox exerts a critical control on organic carbon-rich sedimentation. This is particularly true for Eastern Mediterranean sapropels where seawater stratification is regarded as a major driving force for oxygen depletion, but in which sulphidic (euxinic) bottom waters occur only sporadically. Here we apply a powerful array of geochemical proxies (Fe and Mo stable isotopes together with Mo/U ratios and redox sensitive trace elements (RSTE)) to the determination of water redox evolution during the deposition of Holocene S1 sapropel and its underlying and overlying sediments (ODP core 967D; 2550 m depth). RSTE are asymmetrically distributed within the sapropel, with peak enrichments occurring in its lower (early) part. Negative correlations are found between δFe57 and both Fe/Al and S wt% in the lower sapropel, and are consistent with the benthic Fe shuttle model Fe enrichment in euxinic basins. MoEF/UEF enrichment factor variations show well defined trends identical to those proposed for open marine settings, in which sub-oxic conditions in the background sediments give way to sulphidic waters at the RSTE peak in the lower sapropel. The most notable features of the Mo isotope profile are ‘atypically’ light values (δMo98/95<-0.7‰) in the lower sapropel. Such light Mo isotope values (relative to sea water δMo98/95=2.3‰) have been related to oxic remobilisation. However, negative correlations between δMo98/95 and Fe/Al, Ba/Al, Mo/Al and S imply that the lowest Mo isotopic compositions are associated with peak reducing conditions. Taken in conjunction with the evidence from the other proxies for a sulphidic water column, the light Mo isotope values in the lower sapropel are best explained by a large isotopic fractionation between sea water molybdate and thiomolybdate species in mildly euxinic bottom waters ([H2S]aq <10 μM). The data from this study thus show that hitherto unrecognised euxinic conditions occur during the early stages of deposition of the

  7. Laser isotope separation

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Boyer, Keith; Greiner, Norman R.

    1988-01-01

    A process and apparatus for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photolysis, photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photolysis, photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium.

  8. Photochemical isotope separation

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

    1987-01-01

    A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

  9. Photochemical isotope separation

    DOEpatents

    Robinson, C.P.; Jensen, R.J.; Cotter, T.P.; Greiner, N.R.; Boyer, K.

    1987-04-28

    A process is described for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium. 8 figs.

  10. Laser isotope separation

    DOEpatents

    Robinson, C.P.; Reed, J.J.; Cotter, T.P.; Boyer, K.; Greiner, N.R.

    1975-11-26

    A process and apparatus for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light is described. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photolysis, photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photolysis, photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium.

  11. Measurement of Radon, Thoron, Isotopic Uranium and Thorium to Determine Occupational and Environmental Exposure and Risk at Fernald Feed Material Production Center

    SciTech Connect

    Naomi H. Harley, Ph.D.

    2004-07-01

    To develop a new and novel area and personal radon/thoron detector for both radon isotopes to better measure the exposure to low airborne concentrations of these gases at Fernald. These measurements are to be used to determine atmospheric dispersion and exposure to radon and thoron prior to and during retrieval and removal of the 4000 Ci of radium in the two silos at Fernald.

  12. Minority Language Rights.

    ERIC Educational Resources Information Center

    O Riagain, Padraig; Shuibhne, Niamh Nic

    1997-01-01

    A survey of literature since 1990 on minority languages and language rights focuses on five issues: definition of minorities; individual vs. collective rights; legal bases for minority linguistic rights; applications and interpretations of minority language rights; and assessments of the impact of minority rights legislation. A nine-item annotated…

  13. [Depleted uranium: radiation and ecological safety aspects].

    PubMed

    Ushakov, I B; Afanas'ev, R V; Berezin, G I; Zuev, V G

    2003-01-01

    The authors have analyzed the ecological, sanitary-and-hygienic and medicobiologic aspects of using the impoverished uranium in armaments and military equipment. The influence of impoverished uranium on human body (600 cases) was studied using medicobiologic investigation. It was shown that the particles of aerosol of mixed uranium oxide cause the radiation and chemical damage of kidneys, lungs and other internals. Uranium's alpha-radiation is very effective in induction of biologic effects during internal irradiation. Taking into account that bone tissue is the critical organ for uranium isotopes the medullar tissue is exposed to alpha-radiation. In the armed conflicts of the last decade wide use of armour-piercing means with elements consisted of impoverished uranium has led to the appearance of new technogenic risk factor for the environment and the man. PMID:12825370

  14. Assessing natural attenuation potential at a uranium (U) in situ recovery site (Rosita, TX, USA) using multiple redox-sensitive isotope systems

    NASA Astrophysics Data System (ADS)

    Basu, A.; Brown, S. T.; Christensen, J. N.; DePaolo, D. J.; Reimus, P. W.; Heikoop, J. M.; Simmons, A. M.; House, B.; Schilling, K.; Johnson, T. M.; Pelizza, M.

    2013-12-01

    The In Situ Recovery (ISR) U mining operation at Rosita, TX, USA, involved oxidative dissolution of U from roll front U deposits. This process mobilized U along with other characteristic elements (e.g., Se) from the roll fronts in their soluble and toxic oxidized forms (e.g., U(VI), Se(VI)). The dissolved U(VI) in groundwater poses significant ecological risk due to its chemical toxicity and must be restored below the existing regulatory limit to minimize the environmental impact of ISR mining. However, the undisturbed sediments downgradient to the roll front deposits are expected to remain reduced. Naturally occurring Fe-minerals (e.g., FeS, siderite, magnetite) and microorganisms in the sediments downgradient to ISR activity can reduce dissolved U(VI) to less toxic and insoluble U(IV) and promote natural attenuation. The reduction of oxyanions of U or Se induces measurable isotopic fractionation that can be used to monitor the natural attenuation by downgradient sediments. Here, we used multiple redox-sensitive isotope systems (U, Se, and S) to detect reducing conditions and natural attenuation of U(VI) at the ISR site. We collected groundwater samples from 26 wells located in the ore body, upgradient and downgradient to the ore body. The δ238U values measured in groundwater samples from 23 wells range from 0.48‰ to -1.66‰ (×0.12‰). A preliminary investigation of 6 groundwater samples shows a variation of δ82Se values from -1.44‰ to 5.24‰ (×0.15‰). The δ34SO4 measurements in groundwater vary from 11.8‰ to -19.9‰. The reduction of Se(VI) and SO42- fractionates the lighter isotopes (i.e., 32S and 76Se) in the reduced product phase rendering the remaining reactants in the groundwater enriched in heavier isotopes. Therefore, the high δ82Se and δ34SO4 values may suggest reduction of Se(VI) and SO42-, respectively. The highest δ238U values are observed in the wells located in the ore body or upgradient to the ore body whereas the downgradient

  15. Uranium 238U/235U isotope ratios as indicators of reduction: Results from an in situ biostimulation experiment at Rifle, Colorado, USA

    SciTech Connect

    Bopp IV, C.J.; Lundstrom, C.C.; Johnson, T.M.; Sanford, R.A.; Long, P.E.; Williams, K.H.

    2010-02-01

    The attenuation of groundwater contamination via chemical reaction is traditionally evaluated by monitoring contaminant concentration through time. However, this method can be confounded by common transport processes (e.g. dilution, sorption). Isotopic techniques bypass the limits of concentration methods, and so may provide improved accuracy in determining the extent of reaction. We apply measurements of {sup 238}U/{sup 235}U to a U bioremediation field experiment at the Rifle Integrated Field Research Challenge Site in Rifle, Colorado (USA). An array of monitoring and injection wells was installed on a 100 m{sup 2} plot where U(VI) contamination was present in the groundwater. Acetate-amended groundwater was injected along an up-gradient gallery to encourage the growth of dissimilatory metal reducing bacteria (e.g. Geobacter species). During amendment, U concentration dropped by an order of magnitude in the experiment plot. We measured {sup 238}U/{sup 235}U in samples from one monitoring well by MC-ICP-MS using a double isotope tracer method. A significant {approx}1.00{per_thousand} decrease in {sup 238}U/{sup 235}U occurred in the groundwater as U(VI) concentration decreased. The relationship between {sup 238}U/{sup 235}U and concentration corresponds approximately to a Rayleigh distillation curve with an effective fractionation factor ({alpha}) of 1.00046. We attribute the observed U isotope fractionation to a nuclear field shift effect during enzymatic reduction of U(VI){sub (aq)} to U(IV){sub (s)}.

  16. URANIUM COMPOSITIONS

    DOEpatents

    Allen, N.P.; Grogan, J.D.

    1959-05-12

    This patent relates to high purity uranium alloys characterized by improved stability to thermal cycling and low thermal neutron absorption. The high purity uranium alloy contains less than 0.1 per cent by weight in total amount of any ore or more of the elements such as aluminum, silicon, phosphorous, tin, lead, bismuth, niobium, and zinc.

  17. ISOTOPE FRACTIONATION PROCESS

    DOEpatents

    Clewett, G.H.; Lee, DeW.A.

    1958-05-20

    A new method is described for isotopic enrichment of uranium. It has been found that when an aqueous acidic solution of ionic tetravalent uraniunn is contacted with chelate complexed tetravalent uranium, the U/sup 238/ preferentially concentrates in the complexed phase while U/sup 235/ concentrates in the ionic phase. The effect is enhanced when the chelate compound is water insoluble and is dissolved in a water-immiscible organic solvent. Cupferron is one of a number of sultable complexing agents, and chloroform is a suitable organic solvent.

  18. RECOVERY OF URANIUM FROM TUNGSTEN

    DOEpatents

    Newnam, K.

    1959-02-01

    A method is presented for the rccovery of uranium which has adhered to tungsten parts in electromagnetic isotope separation apparatus. Such a tungsten article is dissolved electrolytically in 20% NaOH by using the tungsten article as the anode. The resulting solution, containing soluble sodium lungstate and an insoluble slime, is then filtered. The slime residue is ignited successively with sodium nitrate and sodium pyrosulfate and leashed, and the resulting filtrates are combined with the original filtrate. Uranium is then recovered from the combined flltrates by diuranate precipitation.

  19. Carbon, Oxygen and Uranium Isotopes in Pedothem Carbonates Reveal Anomalous North American Atmospheric Circulation 70,000 to 55,000 Years Ago

    NASA Astrophysics Data System (ADS)

    Oerter, E.; Sharp, W. D.; Oster, J. L.; Ebeling, A.; Valley, J. W.; Kozdon, R.; Orland, I. J.; Hellstrom, J. C.; Woodhead, J. D.; Hergt, J.; Chadwick, O.; Amundson, R.

    2015-12-01

    Climate conditions in North America during the past two glacial cycles remain uncertain in part because long, well-dated, continuous paleoclimate records are limited in number and sparsely distributed. Here we present the first continuous, millennial resolution paleoclimate proxy record derived from C, O and U isotopes in mm-thick pedogenic carbonate clast-coatings (pedothems), which are widely distributed in semi-arid to arid regions worldwide. Carbonate 230Th/U ages were obtained from laser ablation ICP-MS spots of 93um diameter size, which also yielded 234U/238Ui proxy values for soil water infiltration and paleoprecipitation. The U-series transects were coupled to δ13C and δ18O values obtained by ion probe on ~10um diameter spots. Modern soil carbonate in the region has δ18O and δ13C values that are similar to the youngest (early Holocene) samples acquired in the laminations, strengthening the interpretation that the carbonate reflects soil isotopic conditions at the time of formation. Our new record from the Wind River Basin in Wyoming spans the last 120,000 years and confirms a previously hypothesized period of increased transport of Gulf of Mexico moisture northward into the continental interior from 70,000 to 55,000 years ago. Such pronounced meridional moisture transport, which contrasts with the dominant zonal transport of Pacific moisture into the North American interior by westerly winds before and after 70,000 to 55,000 years ago, may have resulted from a persistent anticyclone developed above the North American ice sheet during Marine Isotope Stage 4. Subsequently, the carbonate record suggests that climate in mid-latitude central North America became progressively more arid during the onset of the last glaciation (both δ13C and 234U/238Ui values become more positive), culminating in peak aridity during the LGM. We conclude that pedothems, when analyzed using micro-analytical techniques, can provide unique insights into past terrestrial climates.

  20. 10 CFR 74.33 - Nuclear material control and accounting for uranium enrichment facilities authorized to produce...

    Code of Federal Regulations, 2014 CFR

    2014-01-01

    ...) Protect against and detect production of uranium enriched to 10 percent or more in the isotope U235; (3... more in the isotope U235 (for centrifuge enrichment facilities this requirement does not apply to each... uranium enriched to 10 percent or more in the isotope U235; and (9) Provide information to aid in...

  1. 10 CFR 74.33 - Nuclear material control and accounting for uranium enrichment facilities authorized to produce...

    Code of Federal Regulations, 2013 CFR

    2013-01-01

    ...) Protect against and detect production of uranium enriched to 10 percent or more in the isotope U235; (3... more in the isotope U235 (for centrifuge enrichment facilities this requirement does not apply to each... uranium enriched to 10 percent or more in the isotope U235; and (9) Provide information to aid in...

  2. 10 CFR 74.33 - Nuclear material control and accounting for uranium enrichment facilities authorized to produce...

    Code of Federal Regulations, 2011 CFR

    2011-01-01

    ...) Protect against and detect production of uranium enriched to 10 percent or more in the isotope U235; (3... more in the isotope U235 (for centrifuge enrichment facilities this requirement does not apply to each... uranium enriched to 10 percent or more in the isotope U235; and (9) Provide information to aid in...

  3. 10 CFR 74.33 - Nuclear material control and accounting for uranium enrichment facilities authorized to produce...

    Code of Federal Regulations, 2012 CFR

    2012-01-01

    ...) Protect against and detect production of uranium enriched to 10 percent or more in the isotope U235; (3... more in the isotope U235 (for centrifuge enrichment facilities this requirement does not apply to each... uranium enriched to 10 percent or more in the isotope U235; and (9) Provide information to aid in...

  4. Uranium-series disequilibrium dating of secondary uranium ore from the south Eastern Desert of Egypt.

    PubMed

    Dawood, Y H

    2001-12-01

    The secondary uranium ore of Um Ara mining area, south Eastern Desert of Egypt, is composed mainly of uranophane and beta-uranophane. They occur in the oxidized zone as idiomorphic crystals filling cavities and as coatings on the fracture surfaces of the alkali-feldspar and albitized granites. The activity ratios 234U/238U and 230Th/234U of the secondary uranium ore and host rocks indicate that there were two main phases of uranium mobility in recent geological time. An earlier precipitation of uranium from solutions forming the secondary ore and a subsequent mobilization resulted in adsorption of uranium to the host granitic rocks. The 230Th/234U age of secondary uranium ore varies from (50 +/- 10) to (159 +/- 69/-45) ka whereas, the age of uranium adsorption to the rocks ranges from (18 +/- 6) to (38 +/- 5) ka. The time of secondary uranium ore precipitation can be attributed to the Saharan II pluvial period which prevailed in Egypt during humid oxygen isotope climatic stage 5. The later uranium mobility and subsequent adsorption by the rocks took place during Kubbaniyan and Nabtian pluvial periods that coincided with oxygen isotope stages 3 and 1, respectively. PMID:11761113

  5. Beneficial Uses of Depleted Uranium

    SciTech Connect

    Brown, C.; Croff, A.G.; Haire, M. J.

    1997-08-01

    Naturally occurring uranium contains 0.71 wt% {sup 235}U. In order for the uranium to be useful in most fission reactors, it must be enriched the concentration of the fissile isotope {sup 235}U must be increased. Depleted uranium (DU) is a co-product of the processing of natural uranium to produce enriched uranium, and DU has a {sup 235}U concentration of less than 0.71 wt%. In the United States, essentially all of the DU inventory is in the chemical form of uranium hexafluoride (UF{sub 6}) and is stored in large cylinders above ground. If this co-product material were to be declared surplus, converted to a stable oxide form, and disposed, the costs are estimated to be several billion dollars. Only small amounts of DU have at this time been beneficially reused. The U.S. Department of Energy (DOE) has begun the Beneficial Uses of DU Project to identify large-scale uses of DU and encourage its reuse for the primary purpose of potentially reducing the cost and expediting the disposition of the DU inventory. This paper discusses the inventory of DU and its rate of increase; DU disposition options; beneficial use options; a preliminary cost analysis; and major technical, institutional, and regulatory issues to be resolved.

  6. Formation and resulfidization of a South Texas roll-type uranium deposit

    USGS Publications Warehouse

    Goldhaber, Martin B.; Reynolds, Richard L.; Rye, Robert O.

    1979-01-01

    iron disulfide phase; and (2) an ore-stage process which led to the development of the uranium roll with emplacement of the characteristic suite of minor and accessory elements and which produced abundant isotopically light marcasite. The host rock was modified by a post-ore stage of resulfidization which precipitated isotopically heavy pyrite. Sulfur isotopic compositions of sulfide and sulfate present in modern ground water within the host sand differ greatly from sulfur isotopic composition of iron disulfides formed during the resulfidization episode. Iron disulfide minerals formed from the sulfur species of modern ground water have not been unequivocally identified.

  7. Isotope Enrichment Detection by Laser Ablation - Laser Absorption Spectrometry: Automated Environmental Sampling and Laser-Based Analysis for HEU Detection

    SciTech Connect

    Anheier, Norman C.; Bushaw, Bruce A.

    2010-01-01

    The global expansion of nuclear power, and consequently the uranium enrichment industry, requires the development of new safeguards technology to mitigate proliferation risks. Current enrichment monitoring instruments exist that provide only yes/no detection of highly enriched uranium (HEU) production. More accurate accountancy measurements are typically restricted to gamma-ray and weight measurements taken in cylinder storage yards. Analysis of environmental and cylinder content samples have much higher effectiveness, but this approach requires onsite sampling, shipping, and time-consuming laboratory analysis and reporting. Given that large modern gaseous centrifuge enrichment plants (GCEPs) can quickly produce a significant quantity (SQ ) of HEU, these limitations in verification suggest the need for more timely detection of potential facility misuse. The Pacific Northwest National Laboratory (PNNL) is developing an unattended safeguards instrument concept, combining continuous aerosol particulate collection with uranium isotope assay, to provide timely analysis of enrichment levels within low enriched uranium facilities. This approach is based on laser vaporization of aerosol particulate samples, followed by wavelength tuned laser diode spectroscopy to characterize the uranium isotopic ratio through subtle differences in atomic absorption wavelengths. Environmental sampling (ES) media from an integrated aerosol collector is introduced into a small, reduced pressure chamber, where a focused pulsed laser vaporizes material from a 10 to 20-µm diameter spot of the surface of the sampling media. The plume of ejected material begins as high-temperature plasma that yields ions and atoms, as well as molecules and molecular ions. We concentrate on the plume of atomic vapor that remains after the plasma has expanded and then cooled by the surrounding cover gas. Tunable diode lasers are directed through this plume and each isotope is detected by monitoring absorbance

  8. Detection of uranium enrichment activities using environmental monitoring techniques

    SciTech Connect

    Belew, W.L.; Carter, J.A.; Smith, D.H.; Walker, R.L.

    1993-03-30

    Uranium enrichment processes have the capability of producing weapons-grade material in the form of highly enriched uranium. Thus, detection of undeclared uranium enrichment activities is an international safeguards concern. The uranium separation technologies currently in use employ UF{sub 6} gas as a separation medium, and trace quantities of enriched uranium are inevitably released to the environment from these facilities. The isotopic content of uranium in the vegetation, soil, and water near the plant site will be altered by these releases and can provide a signature for detecting the presence of enriched uranium activities. This paper discusses environmental sampling and analytical procedures that have been used for the detection of uranium enrichment facilities and possible safeguards applications of these techniques.

  9. Uranium in the environment: occurrence, transfer, and biological effects.

    PubMed

    Ribera, D; Labrot, F; Tisnerat, G; Narbonne, J F

    1996-01-01

    The assessment of uranium chemical and radiological consequences depends on the physicochemical properties of these radioelements and the knowledge of their environmental fate. Although uranium is the source of all these fissionable isotopes, its fate in ecosystems has been poorly investigated. In this review, we have updated information concerning the fate of uranium in the different compartments of the environment, the possibility of transfer to man through the food chain, and the biological and toxicological effects of this metal at cellular, tissular, or organism levels. The physicochemical characteristics of uranium, as well as its regulatory statutes, were reviewed. The fate of uranium in the environment was presented by indicating sources of uranium emission and the possible routes of transfer to man. The biological alterations caused by uranium exposure were discussed, and finally, we presented results collected during our recent study. Some propositions on research to be done to advance the understanding of uranium occurrence in the environment were also given. PMID:8714221

  10. Analysis of solid uranium samples using a small mass spectrometer

    NASA Astrophysics Data System (ADS)

    Kahr, Michael S.; Abney, Kent D.; Olivares, José A.

    2001-07-01

    A mass spectrometer for isotopic analysis of solid uranium samples has been constructed and evaluated. This system employs the fluorinating agent chlorine trifluoride (ClF 3) to convert solid uranium samples into their volatile uranium hexafluorides (UF 6). The majority of unwanted gaseous byproducts and remaining ClF 3 are removed from the sample vessel by condensing the UF 6 and then pumping away the unwanted gases. The UF 6 gas is then introduced into a quadrupole mass spectrometer and ionized by electron impact ionization. The doubly charged bare metal uranium ion (U 2+) is used to determine the U 235/U 238 isotopic ratio. Precision and accuracy for several isotopic standards were found to be better than 12%, without further calibration of the system. The analysis can be completed in 25 min from sample loading, to UF 6 reaction, to mass spectral analysis. The method is amenable to uranium solid matrices, and other actinides.

  11. JACKETING URANIUM

    DOEpatents

    Saller, H.A.; Keeler, J.R.

    1959-07-14

    The bonding to uranium of sheathing of iron or cobalt, or nickel, or alloys thereof is described. The bonding is accomplished by electro-depositing both surfaces to be joined with a coating of silver and amalgamating or alloying the silver layer with mercury or indium. Then the silver alloy is homogenized by exerting pressure on an assembly of the uranium core and the metal jacket, reducing the area of assembly and heating the assembly to homogenize by diffusion.

  12. Analysis of Uranium and Plutonium by MC-ICPMS

    SciTech Connect

    Williams, R W

    2005-02-23

    This procedure is written as general guidance for the measurement of elemental isotopic composition by plasma-source inorganic mass spectrometry. Analytical methods for uranium and plutonium are given as examples.

  13. Depleted Uranium in Repositories

    SciTech Connect

    Haire, M.J.; Croff, A.G.

    1997-12-31

    For uranium to be useful in most fission nuclear reactors, it must be enriched (i.e. the concentration of the fissile isotope 235U must be increased). Therefore, depleted uranium (DU)-uranium which has less than naturally occurring concentrations of 235U-is a co-product of the enrichment process. Four to six tons of DU exist for every ton of fresh light water reactor fuel. There were 407,006 MgU 407,000 metric tons (t) of DU stored on U.S. Department of Energy (DOE) sites as of July 1993. If this DU were to be declared surplus, converted to a stable oxide form, and emplaced in a near surface disposal facility, the costs are estimated to be several billion dollars. However, the U.S. Nuclear Regulatory Commission has stated that near surface disposal of large quantities of DU tails is not appropriate. Thus, there is the possibility that disposition via disposal will be in a deep geological repository. One alternative that may significantly reduce the cost of DU disposition is to use it beneficially. In fact, DOE has begun the Beneficial Uses of DU Project to identify large scale uses of DU and to encourage its reuse. Several beneficial uses, many of which involve applications in the repository per se or in managing the wastes to go into the repository, are discussed in this report.

  14. In-line assay monitor for uranium hexafluoride

    DOEpatents

    Wallace, S.A.

    1980-03-21

    An in-line assay monitor for determining the content of uranium-235 in a uranium hexafluoride gas isotopic separation system is provided which removes the necessity of complete access to the operating parameters of the system for determining the uranium-235 content. The method and monitor for carrying out the method involve cooling of a radiation pervious chamber connected in fluid communication with the selected point in the system to withdraw a specimen and solidify the specimen in the chamber. The specimen is irradiated by means of an ionizing radiation source of energy different from that of the 185 keV gamma emissions from uranium-235. The uranium-235 content of the specimen is determined from comparison of the accumulated 185 keV energy counts and reference energy counts. The latter is used to measure the total uranium isotopic content of the specimen.

  15. Continuous reduction of uranium tetrafluoride

    SciTech Connect

    DeMint, A.L.; Maxey, A.W.

    1993-10-21

    Operation of a pilot-scale system for continuous metallothermic reduction of uranium tetrafluoride (UF{sub 4} or green salt) has been initiated. This activity is in support of the development of a cost- effective process to produce uranium-iron (U-Fe) alloy feed for the Uranium-Atomic Vapor Laser Isotope Separation (U-AVLIS) program. To date, five runs have been made to reduce green salt (UF{sub 4}) with magnesium. During this quarter, three runs were made to perfect the feeding system, examine feed rates, and determine the need for a crust breaker/stirrer. No material was drawn off in any of the runs; both product metal and by-product salt were allowed to accumulate in the reactor.

  16. Isotope separation and advanced manufacturing technology

    NASA Astrophysics Data System (ADS)

    Carpenter, J.; Kan, T.

    This is the fourth issue of a semiannual report for the Isotope Separation and Advanced Materials Manufacturing (ISAM) Technology Program at Lawrence Livermore National Laboratory. Primary objectives include: (1) the Uranium Atomic Vapor Laser Isotope Separation (UAVLIS) process, which is being developed and prepared for deployment as an advanced uranium enrichment capability; (2) Advanced manufacturing technologies, which include industrial laser and E-beam material processing and new manufacturing technologies for uranium, plutonium, and other strategically important materials in support of DOE and other national applications. This report features progress in the ISAM Program from October 1993 through March 1994.

  17. URANIUM-SERIES CONSTRAINTS ON RADIONUCLIDE TRANSPORT AND GROUNDWATER FLOW AT NOPAL I URANIUM DEPOSIT, SIERRA PENA BLANCA, MEXICO

    SciTech Connect

    S. J. Goldstein, S. Luo, T. L. Ku, and M. T. Murrell

    2006-04-01

    Uranium-series data for groundwater samples from the vicinity of the Nopal I uranium ore deposit are used to place constraints on radionuclide transport and hydrologic processes at this site, and also, by analogy, at Yucca Mountain. Decreasing uranium concentrations for wells drilled in 2003 suggest that groundwater flow rates are low (< 10 m/yr). Field tests, well productivity, and uranium isotopic constraints also suggest that groundwater flow and mixing is limited at this site. The uranium isotopic systematics for water collected in the mine adit are consistent with longer rock-water interaction times and higher uranium dissolution rates at the front of the adit where the deposit is located. Short-lived nuclide data for groundwater wells are used to calculate retardation factors that are on the order of 1,000 for radium and 10,000 to 10,000,000 for lead and polonium. Radium has enhanced mobility in adit water and fractures near the deposit.

  18. Minority Women's Health

    MedlinePlus

    ... migrant issues Access to health care Language barriers Human trafficking Taking care of your health Immunizations and screenings Sharing family health history Health before pregnancy More... Government in action on minority women's health Minority partnerships ...

  19. Minority Inclusion Programs.

    ERIC Educational Resources Information Center

    Gelfand, M. David

    1995-01-01

    Asserts that the United States has a long, sad history of discrimination against minority rights. Discusses the origins and history of minority inclusion or affirmative action programs. Includes a special report on the "English Only" movement. (CFR)

  20. Ethnic Minorities and Telecommunications.

    ERIC Educational Resources Information Center

    Hayes-Hull, Marion

    Developments in communications technology should become a major concern of minorities (native Americans and Americans of African, Asian, and Hispanic racial or ethnic origin). Although minorities are disillusioned with broadcast television because television decision makers have not been sensitive to minority needs, they have shown interest…

  1. Alcohol and Minority Youth.

    ERIC Educational Resources Information Center

    Wright, Roosevelt, Jr.; Watts, Thomas D.

    1991-01-01

    Maintains that minority youth who use (or abuse) alcohol in American society deal with using alcohol, being minority, and being young, three dimensions viewed by society with mixed, sometimes hostile and/or fearful reactions. Suggests that examining alcoholism among minority youth involves coming to grips with poverty, education, income, and life…

  2. Tramp uranium

    SciTech Connect

    Hendrixson, E.S.; Williamson, T.G.

    1988-01-01

    Many utilities have implemented a no leaker philosophy for fuel performance and actively pursue removing leaking fuel assemblies from their reactor cores whenever a leaking fuel assembly is detected. Therefore, the only source for fission product activity in the RCS when there are no leaking fuel assemblies is tramp uranium. A technique has been developed that strips uranium impurities from ZrCl{sub 4}. Unless efforts are made to remove natural uranium impurities from reactor materials, the utilities will not be able to reduce the RCS specific {sup 131}I activity in PWRs to below the lower limit of {approximately}1.0 x 10{minus{sup 4}} {mu}Ci/g.

  3. The Nabarlek uranium deposit, Northern Territory, Australia: Some petrologic and geochemical constraints on genesis

    SciTech Connect

    Ewers, G.R.; Donnelly, T.M.; Ferguson, J.

    1983-08-01

    The Nabarlek uranium deposit, Northern Territory, Australia, is confined to a shear zone in contorted and metasomatized early Proterozoic schists and occurs near an unconformity with overlying middle Proterozoic sandstone. Massive chlorite + or - sericite + or - hematite rocks, breccias, and intensely altered schists are characteristic of the ore zone, and at least three generations of chlorite have been recognized and described. The primary ore mineral assemblage is dominated by uraninite intergrown with chlorite. The orebody was sericitized at or after 920 m.y. ago, resulting in the widespread replacement and breakdown of chlorite, the formation of hematite, and the solution and redeposition of uraninite. Redox reactions involving iron and uranium are evident in sericitized rocks containing hematite and residual uraninite. High U/Th ratios in the ore zone suggest that uranium was transported to the site of deposition as a uranyl complex. Although no carbonaceous material occurs in the ore zone, isotopic data on minor carbonate associated with uraninite suggest that organic material was originally associated with the mineralization and indicate that these carbonates have evolved from the interaction of hydrothermal fluids with this material. Erosion of the middle Proterozoic cover rocks in the recent past has exposed the deposit to the effects of weathering.

  4. Detection of depleted uranium in urine of veterans from the 1991 Gulf War.

    PubMed

    Gwiazda, R H; Squibb, K; McDiarmid, M; Smith, D

    2004-01-01

    American soldiers involved in "friendly fire" accidents during the 1991 Gulf War were injured with depleted-uranium-containing fragments or possibly exposed to depleted uranium via other routes such as inhalation, ingestion, and/or wound contamination. To evaluate the presence of depleted uranium in these soldiers eight years later, the uranium concentration and depleted uranium content of urine samples were determined by inductively coupled plasma mass spectrometry in (a) depleted uranium exposed soldiers with embedded shrapnel, (b) depleted uranium exposed soldiers with no shrapnel, and (c) a reference group of deployed soldiers not involved in the friendly fire incidents. Uranium isotopic ratios measured in many urine samples injected directly into the inductively coupled plasma mass spectrometer and analyzed at a mass resolution m/delta m of 300 appeared enriched in 235U with respect to natural abundance (0.72%) due to the presence of an interference of a polyatomic molecule of mass 234.81 amu that was resolved at a mass resolution m/delta m of 4,000. The 235U abundance measured on uranium separated from these urines by anion exchange chromatography was clearly natural or depleted. Urine uranium concentrations of soldiers with shrapnel were higher than those of the two other groups, and 16 out of 17 soldiers with shrapnel had detectable depleted uranium in their urine. In depleted uranium exposed soldiers with no shrapnel, depleted uranium was detected in urine samples of 10 out of 28 soldiers. The median uranium concentration of urines with depleted uranium from soldiers without shrapnel was significantly higher than in urines with no depleted uranium, though substantial overlap in urine uranium concentrations existed between the two groups. Accordingly, assessment of depleted uranium exposure using urine must rely on uranium isotopic analyses, since urine uranium concentration is not an unequivocal indicator of depleted uranium presence in soldiers with no

  5. Isotope separation by laser technology

    NASA Astrophysics Data System (ADS)

    Stoll, Wolfgang

    2002-03-01

    Isotope separation processes operate on very small differences, given either by the Quotient of masses with the same number of electrons or by their mass difference. When separating isotopes of light elements in mass quantities, thermodynamic processes accounting for the quotient, either in diffusion, chemical reactivity or distillation are used. For heavy elements those quotients are very small. Therefore they need a large number of separation steps. Large plants with high energy consumption result from that. As uranium isotope separation is the most important industrial field, alternatives, taking account for the mass difference, as e.g. gas centrifuges, have been developed. They use only a fraction of the energy input, but need a very large number of machines, as the individual throughput is small. Since it was discovered, that molecules of high symmetry like Uranium-Hexafluoride as a deep-cooled gas stream can be ionized by multiple photon excitation, this process was studied in detail and in competition to the selective ionization of metal vapors, as already demonstrated with uranium. The paper reports about the principles of the laser excitation for both processes, the different laboratory scale and prototypical plants built, the difficulties with materials, as far as the metal vapor laser separation is concerned, and the difficulties experienced in the similarity in molecular spectra. An overview of the relative economic merits of the different processes and the auspices in a saturated market for uranium isotope separation, together with other potential markets for molecular laser separation, is contained in the conclusions.

  6. Uranium bombs

    NASA Astrophysics Data System (ADS)

    DeGroot, Gerard

    2009-11-01

    Enrico Fermi was a brilliant physicist, but he did occasionally get things wrong. In 1934 he famously bombarded a sample of uranium with neutrons. The result was astounding: the experiment had, Fermi concluded, produced element 93, later called neptunium. The German physicist Ida Noddack, however, came to an even more spectacular conclusion, namely that Fermi had split the uranium nucleus to produce lighter elements. Noddack's friend Otto Hahn judged that idea preposterous and advised her to keep quiet, since ridicule could ruin a female physicist. She ignored that advice, and was, indeed, scorned.

  7. The timing of sea-level high-stands during Marine Isotope Stages 7.5 and 9: Constraints from the uranium-series dating of fossil corals from Henderson Island

    NASA Astrophysics Data System (ADS)

    Andersen, Morten B.; Stirling, Claudine H.; Potter, Emma-Kate; Halliday, Alex N.; Blake, Steve G.; McCulloch, Malcolm T.; Ayling, Bridget F.; O'Leary, Michael J.

    2010-06-01

    Direct dating of fossil coral reefs using the U-series chronometer provides an important independent test of the Milankovitch orbital forcing theory of climate change. However, well-dated fossil corals pre-dating the last interglacial period (>130 thousand years ago; ka) are scarce due to, (1) a lack of sampling localities, (2) insufficient analytical precision in U-series dating methods, and (3) diagenesis which acts to violate the assumption of closed-system U-series isotopic decay in fossil corals. Here we present 50 new high-precision U-series age determinations for fossil corals from Henderson Island, an emergent coral atoll in the central South Pacific. U-series age determinations associated with the Marine Isotope Stage (MIS) 9 interglacial and MIS 7.5 interstadial periods are reported. The fossil corals show relatively little open-system U-series behaviour in comparison to other localities with fossil coral reefs formed prior to the last glacial cycle, however, open-system U-series behaviour is still evident in most of the dated corals. In particular, percent-level shifts in the [ 230Th/ 238U] act composition are observed, leading to conventional U-series ages that are significantly younger or older than the true sample age. This open-system U-series behaviour is not accounted for by any of the open-system U-series models, indicating that new models should be derived. The new U-series ages reported here support and extend earlier findings reported in Stirling et al. (2001), providing evidence of prolific coral reef development on Henderson Island at ˜320 ka, most likely correlated with MIS 9.3, and subsequent reef development at ˜307 ka during MIS 9.1, while relative sea-level was potentially ˜20 m lower than during MIS 9.3. The U-series ages for additional well-preserved fossil corals are suggestive of minor reef development on Henderson Island during MIS 7.5 (245-230 ka) at 240.3 ± 0.8 and 234.7 ± 1.3 ka. All U-series observations are consistent with

  8. Machining of uranium and uranium alloys

    SciTech Connect

    Morris, T.O.

    1981-12-14

    Uranium and uranium alloys can be readily machined by conventional methods in the standard machine shop when proper safety and operating techniques are used. Material properties that affect machining processes and recommended machining parameters are discussed. Safety procedures and precautions necessary in machining uranium and uranium alloys are also covered. 30 figures.

  9. Uranium, natural

    Integrated Risk Information System (IRIS)

    Uranium , natural ; CASRN 7440 - 61 - 1 Human health assessment information on a chemical substance is included in the IRIS database only after a comprehensive review of toxicity data , as outlined in the IRIS assessment development process . Sections I ( Health Hazard Assessments for Noncarcinogeni

  10. URANIUM ALLOYS

    DOEpatents

    Seybolt, A.U.

    1958-04-15

    Uranium alloys containing from 0.1 to 10% by weight, but preferably at least 5%, of either zirconium, niobium, or molybdenum exhibit highly desirable nuclear and structural properties which may be improved by heating the alloy to about 900 d C for an extended period of time and then rapidly quenching it.

  11. Isotope separation by laser means

    DOEpatents

    Robinson, C. Paul; Jensen, Reed J.; Cotter, Theodore P.; Greiner, Norman R.; Boyer, Keith

    1982-06-15

    A process for separating isotopes by selective excitation of isotopic species of a volatile compound by tuned laser light. A highly cooled gas of the volatile compound is produced in which the isotopic shift is sharpened and defined. Before substantial condensation occurs, the cooled gas is irradiated with laser light precisely tuned to a desired wavelength to selectively excite a particular isotopic species in the cooled gas. The laser light may impart sufficient energy to the excited species to cause it to undergo photochemical reaction or even to photoionize. Alternatively, a two-photon irradiation may be applied to the cooled gas to induce photochemical reaction or photoionization. The process is particularly applicable to the separation of isotopes of uranium and plutonium.

  12. Uranium industry annual 1996

    SciTech Connect

    1997-04-01

    The Uranium Industry Annual 1996 (UIA 1996) provides current statistical data on the US uranium industry`s activities relating to uranium raw materials and uranium marketing. The UIA 1996 is prepared for use by the Congress, Federal and State agencies, the uranium and nuclear electric utility industries, and the public. Data on uranium raw materials activities for 1987 through 1996 including exploration activities and expenditures, EIA-estimated reserves, mine production of uranium, production of uranium concentrate, and industry employment are presented in Chapter 1. Data on uranium marketing activities for 1994 through 2006, including purchases of uranium and enrichment services, enrichment feed deliveries, uranium fuel assemblies, filled and unfilled market requirements, uranium imports and exports, and uranium inventories are shown in Chapter 2. A feature article, The Role of Thorium in Nuclear Energy, is included. 24 figs., 56 tabs.

  13. Magnitude and variability of disequilibrium in San Antonio Valley uranium deposit, Valencia County

    SciTech Connect

    Moore, S.C.; Lavery, N.G.

    1980-01-01

    The San Antonio Valley deposit is elongate northwest-southeast, is approximately 1 mile long and 1,000 wide and averages 6 to 12 ft in thickness. This trend-type deposit has a chemically reduced mineralogy and occurs below the water table. The average disequilibrium factor for the deposit shows a 6 percent enrichment in chemical uranium; however, systematic variations occur throughout the deposit. The northeastern edge averages 14 percent excessive chemical uranium relative to equivalent uranium, and the southwestern edge is deficient in chemical uranium. Instead of applying a single correction factor to the ore reserves calculated from radiometric data, three correction factors can be used, one for each of the three northwest-southeast elongate zones. The use of multiple correction factors can improve mine planning and should increase the total amount of uranium recovered from the deposit. Vertical profiles of chemical uranium and closed-can equivalent uranium through mineralized intervals suggest dispersion of uranium daughter isotopes away from uranium concentrations in some core holes and deposition of daughter isotopes in other core holes. Horizontal data plots suggest that depletion of daughter isotopes is pronounced along the northeast edge of the deposit and that their redeposition occurs in the central and soutwest parts. Groundwater flow from northeast to southwest through the deposit may have caused the transport and redeposition of the daughter isotopes, which in turn created the longitudinal zones of uranium excess and deficiency. This flow system caused both the local migration of daughter isotopes away from uranium concentrations seen in drill cores and also the larger scale transport of daughter isotopes in the direction of the hydrologic gradient. This model is based on chemical-uranium assays and on closed-can equivalent-uranium assays.

  14. Innovations in Mass Spectrometry for Precise and Accurate Isotope Ratio Determination from Very Small Analyte Quantities (Invited)

    NASA Astrophysics Data System (ADS)

    Lloyd, N. S.; Bouman, C.; Horstwood, M. S.; Parrish, R. R.; Schwieters, J. B.

    2010-12-01

    This presentation describes progress in mass spectrometry for analysing very small analyte quantities, illustrated by example applications from nuclear forensics. In this challenging application, precise and accurate (‰) uranium isotope ratios are required from 1 - 2 µm diameter uranium oxide particles, which comprise less than 40 pg of uranium. Traditionally these are analysed using thermal ionisation mass spectrometry (TIMS), and more recently using secondary ionisation mass spectrometry (SIMS). Multicollector inductively-coupled plasma mass spectrometry (MC-ICP-MS) can offer higher productivity compared to these techniques, but is traditionally limited by low efficiency of analyte utilisation (sample through to ion detection). Samples can either be introduced as a solution, or sampled directly from solid using laser ablation. Large multi-isotope ratio datasets can help identify provenance and intended use of anthropogenic uranium and other nuclear materials [1]. The Thermo Scientific NEPTUNE Plus (Bremen, Germany) with ‘Jet Interface’ option offers unparalleled MC-ICP-MS sensitivity. An analyte utilisation of c. 4% has previously been reported for uranium [2]. This high-sensitivity configuration utilises a dry high-capacity (100 m3/h) interface pump, special skimmer and sampler cones and a desolvating nebuliser system. Coupled with new acquisition methodologies, this sensitivity enhancement makes possible the analysis of micro-particles and small sample volumes at higher precision levels than previously achieved. New, high-performance, full-size and compact discrete dynode secondary electron multipliers (SEM) exhibit excellent stability and linearity over a large dynamic range and can be configured to simultaneously measure all of the uranium isotopes. Options for high abundance-sensitivity filters on two ion beams are also available, e.g. for 236U and 234U. Additionally, amplifiers with high ohm (1012 - 1013) feedback resistors have been developed to

  15. Basic characterization of highly enriched uranium by gamma spectrometry

    NASA Astrophysics Data System (ADS)

    Nguyen, Cong Tam; Zsigrai, József

    2006-05-01

    Gamma-spectrometric methods suitable for the characterization of highly enriched uranium samples encountered in illicit trafficking of nuclear materials are presented. In particular, procedures for determining the 234U, 235U, 238U, 232U and 236U contents and the age of highly enriched uranium are described. Consequently, the total uranium content and isotopic composition can be calculated. For determining the 238U and 232U contents a low-background chamber was used. In addition, age dating of uranium was also performed using low-background spectrometry.

  16. Model Minority Stereotype Reconsidered.

    ERIC Educational Resources Information Center

    Kobayashi, Futoshi

    This paper explores the origin and historical background of the "model minority" stereotype. It includes evidence illustrating problems resulting from the artificial grouping of Asian Americans as one ethnic group and the stereotype's influence on young Asian Americans. In the 1960s, the U.S. media began to portray the model minority through…

  17. Minorities in Higher Education.

    ERIC Educational Resources Information Center

    Justiz, Manuel J., Ed.; And Others

    This book presents 19 papers on efforts to increase the participation of members of minority groups in higher education. The papers are: (1) "Demographic Trends and the Challenges to American Higher Education" (Manuel Justiz); (2) "Three Realities: Minority Life in the United States--The Struggle for Economic Equity (adapted by Don M. Blandin);…

  18. Recruiting Minority Students.

    ERIC Educational Resources Information Center

    Reed, Bobette P.; Dandridge, William L.

    To help improve private schools' recruitment of minority students, this handbook discusses where and how to begin, recruitment strategies, applicant assessment, and the need for in-school support systems for minority students. The authors stress that each school should begin by analyzing its own objectives, attitudes, and admission program.…

  19. Gerontology Training for Minorities.

    ERIC Educational Resources Information Center

    Cho, Pill Jay

    The Grambling State University Minority Management Internship in Aging program described in this report was designed to provide internships to social work students to aid the minority elderly. The status of the elderly in the United States and the personnel and agencies that assist them are discussed in the following chapters: (1) "Introduction"…

  20. American Minorities in Astronomy.

    ERIC Educational Resources Information Center

    Price, Jill S.; Hafer, Abigail A.

    1995-01-01

    A collection of articles that address the question of why minorities are still underrepresented in science after years of civil rights legislation and affirmative action. A variety of programs aimed at increasing minorities and women in the field of astronomy and other sciences are discussed. Personal accounts are also provided. (LZ)

  1. Minority Achievement Report.

    ERIC Educational Resources Information Center

    Prince George's Community Coll., Largo, MD. Office of Institutional Research and Analysis.

    This report summarizes the achievements of Prince George's Community College (PGCC) with regard to minority outcomes. Table 1 summarizes the undergraduate enrollment trends for African Americans as well as total minorities from fall 1994 through fall 1998. Both the headcount number of African American students and the proportion of African…

  2. Derived enriched uranium market

    SciTech Connect

    Rutkowski, E.

    1996-12-01

    The potential impact on the uranium market of highly enriched uranium from nuclear weapons dismantling in the Russian Federation and the USA is analyzed. Uranium supply, conversion, and enrichment factors are outlined for each country; inventories are also listed. The enrichment component and conversion components are expected to cause little disruption to uranium markets. The uranium component of Russian derived enriched uranium hexafluoride is unresolved; US legislation places constraints on its introduction into the US market.

  3. The local minority game

    NASA Astrophysics Data System (ADS)

    Moelbert, S.; De Los Rios, P.

    2002-01-01

    Ecologists and economists try to explain collective behavior in terms of competitive systems of selfish individuals with the ability to learn from the past. Statistical physicists have been investigating models which might contribute to the understanding of the underlying mechanisms of these systems. During the last 3 yr one intuitive model, commonly referred to as the minority game (MG), has attracted considerable attention. Powerful yet simple, the minority game has produced encouraging results which can explain the temporal behavior of competitive systems. Here we switch the interest to the phenomena due to a distribution of the individuals in space. For analyzing these effects we modify the minority game and the local minority game (LMG) is introduced. We study the system both numerically and analytically, using the customary techniques already developed for the ordinary Minority Game.

  4. Isotopic Biogeochemistry

    NASA Technical Reports Server (NTRS)

    Hayes, J. M.

    1985-01-01

    An overview is provided of the biogeochemical research. The funding, productivity, personnel and facilities are reviewed. Some of the technical areas covered are: carbon isotopic records; isotopic studies of banded iron formations; isotope effects in microbial systems; studies of organic compounds in ancient sediments; and development in isotopic geochemistry and analysis.

  5. Uranium Industry Annual, 1992

    SciTech Connect

    Not Available

    1993-10-28

    The Uranium Industry Annual provides current statistical data on the US uranium industry for the Congress, Federal and State agencies, the uranium and electric utility industries, and the public. The feature article, ``Decommissioning of US Conventional Uranium Production Centers,`` is included. Data on uranium raw materials activities including exploration activities and expenditures, resources and reserves, mine production of uranium, production of uranium concentrate, and industry employment are presented in Chapter 1. Data on uranium marketing activities including domestic uranium purchases, commitments by utilities, procurement arrangements, uranium imports under purchase contracts and exports, deliveries to enrichment suppliers, inventories, secondary market activities, utility market requirements, and uranium for sale by domestic suppliers are presented in Chapter 2.

  6. 31 CFR 540.317 - Uranium feed; natural uranium feed.

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 31 Money and Finance:Treasury 3 2011-07-01 2011-07-01 false Uranium feed; natural uranium feed...) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The term uranium feed or natural uranium feed means natural uranium in the form of UF6 suitable for...

  7. 31 CFR 540.317 - Uranium feed; natural uranium feed.

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 31 Money and Finance: Treasury 3 2010-07-01 2010-07-01 false Uranium feed; natural uranium feed...) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed. The term uranium feed or natural uranium feed means natural uranium in the form of UF6 suitable for...

  8. URANIUM EXTRACTION

    DOEpatents

    Harrington, C.D.; Opie, J.V.

    1958-07-01

    The recovery of uranium values from uranium ore such as pitchblende is described. The ore is first dissolved in nitric acid, and a water soluble nitrate is added as a salting out agent. The resulting feed solution is then contacted with diethyl ether, whereby the bulk of the uranyl nitrate and a portion of the impurities are taken up by the ether. This acid ether extract is then separated from the aqueous raffinate, and contacted with water causing back extractioa of the uranyl nitrate and impurities into the water to form a crude liquor. After separation from the ether extract, this crude liquor is heated to about 118 deg C to obtain molten uranyl nitrate hexahydratc. After being slightly cooled the uranyl nitrate hexahydrate is contacted with acid free diethyl ether whereby the bulk of the uranyl nitrate is dissolved into the ethcr to form a neutral ether solution while most of the impurities remain in the aqueous waste. After separation from the aqueous waste, the resultant ether solution is washed with about l0% of its volume of water to free it of any dissolved impurities and is then contacted with at least one half its volume of water whereby the uranyl nitrate is extracted into the water to form an aqueous product solution.

  9. NIH Minority Programs.

    ERIC Educational Resources Information Center

    National Institutes of Health (DHHS), Bethesda, MD.

    This publication contains brief descriptions of National Institutes of Health programs for underrepresented minorities, including fellowships, programs for high school students, graduate research assistantships, postdoctoral training, and programs for college students. The publication provides a description of each program, eligibility…

  10. Minority Women's Health: Latinas

    MedlinePlus

    ... left navigation Minority Women's Health African-Americans Latinas Asian-Americans Native Hawaiians and other Pacific Islanders American Indians/ ... Rican, South or Central American, or other Spanish culture or origin. Latinos may be any race. This ...

  11. Minority workers and communities.

    PubMed

    Frumkin, H; Walker, E D; Friedman-Jiménez, G

    1999-01-01

    Environmental and occupational hazards do not affect all communities equally. Members of ethnic and racial minorities, whether as working people or as community residents, sustain disproportionate risks from chemical, physical, and biological hazards. This paper reviews the nature of these disproportionate risks, focusing primarily on the workplace, but considering general environmental exposures as well. It discusses three principal mechanisms of increased risk: excessive hazardous exposures in both the workplace and the general environment, increased susceptibility, and inferior healthcare. It presents evidence that, as the result of these factors, members of minority groups display elevated rates of work-related illness, injury, fatality, and disability. Finally, it offers recommendations with regard to research, primary prevention, minority recruitment into the occupational health professions, and treatment and compensation for injured and ill minority workers. PMID:10378973

  12. Minority Innovation Challenges Institute

    NASA Video Gallery

    Do you want to learn more about how to compete in NASA’s technical challenges for both prestige and significant cash prizes? NASA’s Minority Innovation Challenges Institute trains and mentors mino...

  13. Uranium in NIMROC standard igneous rock samples

    NASA Technical Reports Server (NTRS)

    Rowe, M. W.; Herndon, J. M.

    1976-01-01

    Results are reported for analysis of the uranium in multiple samples of each of six igneous-rock standards (dunite, granite, lujavrite, norite, pyroxenite, and syenite) prepared as geochemical reference standards for elemental and isotopic compositions. Powdered rock samples were examined by measuring delayed neutron emission after irradiation with a flux of the order of 10 to the 13th power neutrons/sq cm per sec in a nuclear reactor. The measurements are shown to compare quite favorably with previous uranium determinations for other standard rock samples.

  14. Multichoice minority game

    SciTech Connect

    Ein-Dor, Liat; Metzler, Richard; Kanter, Ido; Kinzel, Wolfgang

    2001-06-01

    The generalization of the problem of adaptive competition, known as the minority game, to the case of K possible choices for each player, is addressed, and applied to a system of interacting perceptrons with input and output units of a type of K-state Potts spins. An optimal solution of this minority game, as well as the dynamic evolution of the adaptive strategies of the players, are solved analytically for a general K and compared with numerical simulations.

  15. PRODUCTION OF URANIUM MONOCARBIDE

    DOEpatents

    Powers, R.M.

    1962-07-24

    A method of making essentially stoichiometric uranium monocarbide by pelletizing a mixture of uranium tetrafluoride, silicon, and carbon and reacting the mixture at a temperature of approximately 1500 to 1700 deg C until the reaction goes to completion, forming uranium monocarbide powder and volatile silicon tetrafluoride, is described. The powder is then melted to produce uranium monocarbide in massive form. (AEC)

  16. PRODUCTION OF URANIUM TETRACHLORIDE

    DOEpatents

    Calkins, V.P.

    1958-12-16

    A process is descrlbed for the production of uranium tetrachloride by contacting uranlum values such as uranium hexafluoride, uranlum tetrafluoride, or uranium oxides with either aluminum chloride, boron chloride, or sodium alumlnum chloride under substantially anhydrous condltlons at such a temperature and pressure that the chlorldes are maintained in the molten form and until the uranium values are completely converted to uranlum tetrachloride.

  17. In-line assay monitor for uranium hexafluoride

    DOEpatents

    Wallace, Steven A.

    1981-01-01

    An in-line assay monitor for determining the content of uranium-235 in a uranium hexafluoride gas isotopic separation system is provided which removes the necessity of complete access to the operating parameters of the system for determining the uranium-235 content. The monitor is intended for uses such as safeguard applications to assure that weapons grade uranium is not being produced in an enrichment cascade. The method and monitor for carrying out the method involve cooling of a radiation pervious chamber connected in fluid communication with the selected point in the system to withdraw a specimen and solidify the specimen in the chamber. The specimen is irradiated by means of an ionizing radiation source of energy different from that of the 185 keV gamma emissions from the uranium-235 present in the specimen. Simultaneously, the gamma emissions from the uranium-235 of the specimen and the source emissions transmitted through the sample are counted and stored in a multiple channel analyzer. The uranium-235 content of the specimen is determined from the comparison of the accumulated 185 keV energy counts and the reference energy counts. The latter is used to measure the total uranium isotopic content of the specimen. The process eliminates the necessity of knowing the system operating conditions and yet obtains the necessary data without need for large scintillation crystals and sophisticated mechanical designs.

  18. Mass-independent isotope effects.

    PubMed

    Buchachenko, Anatoly L

    2013-02-28

    Three fundamental properties of atomic nuclei-mass, spin (and related magnetic moment), and volume-are the source of isotope effects. The mostly deserved and popular, with almost hundred-year history, is the mass-dependent isotope effect. The first mass-independent isotope effect which chemically discriminates isotopes by their nuclear spins and nuclear magnetic moments rather than by their masses was detected in 1976. It was named as the magnetic isotope effect because it is controlled by magnetic interaction, i.e., electron-nuclear hyperfine coupling in the paramagnetic species, the reaction intermediates. The effect follows from the universal physical property of chemical reactions to conserve angular momentum (spin) of electrons and nuclei. It is now detected for oxygen, silicon, sulfur, germanium, tin, mercury, magnesium, calcium, zinc, and uranium in a great variety of chemical and biochemical reactions including those of medical and ecological importance. Another mass-independent isotope effect was detected in 1983 as a deviation of isotopic distribution in reaction products from that which would be expected from the mass-dependent isotope effect. On the physical basis, it is in fact a mass-dependent effect, but it surprisingly results in isotope fractionation which is incompatible with that predicted by traditional mass-dependent effects. It is supposed to be a function of dynamic parameters of reaction and energy relaxation in excited states of products. The third, nuclear volume mass-independent isotope effect is detected in the high-resolution atomic and molecular spectra and in the extraction processes, but there are no unambiguous indications of its importance as an isotope fractionation factor in chemical reactions. PMID:23301791

  19. DECONTAMINATION OF URANIUM

    DOEpatents

    Feder, H.M.; Chellew, N.R.

    1958-02-01

    This patent deals with the separation of rare earth and other fission products from neutron bombarded uranium. This is accomplished by melting the uranium in contact with either thorium oxide, maguesium oxide, alumnum oxide, beryllium oxide, or uranium dioxide. The melting is preferably carried out at from 1150 deg to 1400 deg C in an inert atmosphere, such as argon or helium. During this treatment a scale of uranium dioxide forms on the uranium whtch contains most of the fission products.

  20. Apparatus for storing hydrogen isotopes

    DOEpatents

    McMullen, John W.; Wheeler, Michael G.; Cullingford, Hatice S.; Sherman, Robert H.

    1985-01-01

    An improved method and apparatus for storing isotopes of hydrogen (especially tritium) are provided. The hydrogen gas(es) is (are) stored as hydrides of material (for example uranium) within boreholes in a block of copper. The mass of the block is critically important to the operation, as is the selection of copper, because no cooling pipes are used. Because no cooling pipes are used, there can be no failure due to cooling pipes. And because copper is used instead of stainless steel, a significantly higher temperature can be reached before the eutectic formation of uranium with copper occurs, (the eutectic of uranium with the iron in stainless steel forming at a significantly lower temperature).

  1. URANIUM DECONTAMINATION

    DOEpatents

    Buckingham, J.S.; Carroll, J.L.

    1959-12-22

    A process is described for reducing the extractability of ruthenium, zirconium, and niobium values into hexone contained in an aqueous nitric acid uranium-containing solution. The solution is made acid-deficient, heated to between 55 and 70 deg C, and at that temperature a water-soluble inorganic thiosulfate is added. By this, a precipitate is formed which carries the bulk of the ruthenium, and the remainder of the ruthenium as well as the zirconium and niobium are converted to a hexone-nonextractable form. The rutheniumcontaining precipitate can either be removed from the solu tion or it can be dissolved as a hexone-non-extractable compound by the addition of sodium dichromate prior to hexone extraction.

  2. Synthesis of Uranium Trichloride for the Pyrometallurgical Processing of Used Nuclear Fuel

    SciTech Connect

    B.R. Westphal; J.C. Price; R.D. Mariani

    2011-11-01

    The pyroprocessing of used nuclear fuel via electrorefining requires the continued addition of uranium trichloride to sustain operations. Uranium trichloride is utilized as an oxidant in the system to allow separation of uranium metal from the minor actinides and fission products. The inventory of uranium trichloride had diminished to a point that production was necessary to continue electrorefiner operations. Following initial experimentation, cupric chloride was chosen as a reactant with uranium metal to synthesize uranium trichloride. Despite the variability in equipment and charge characteristics, uranium trichloride was produced in sufficient quantities to maintain operations in the electrorefiner. The results and conclusions from several experiments are presented along with a set of optimized operating conditions for the synthesis of uranium trichloride.

  3. Intense alpha-particle emitting crystallites in uranium mill wastes

    USGS Publications Warehouse

    Landa, E.R.; Stieff, L.R.; Germani, M.S.; Tanner, A.B.; Evans, J.R.

    1994-01-01

    Nuclear emulsion microscopy has demonstrated the presence of small, intense ??-particle emitting crystallites in laboratory-produced tailings derived from the sulfuric acid milling of uranium ores. The ??-particle activity is associated with the isotope pair 210Pb 210Po, and the host mineral appears to be PbSO4 occurring as inclusions in gypsum laths. These particles represent potential inhalation hazards at uranium mill tailings disposal areas. ?? 1994.

  4. Isotopic anomalies in extraterrestrial grains.

    PubMed

    Ireland, T R

    1996-03-01

    Isotopic compositions are referred to as anomalous if the isotopic ratios measured cannot be related to the terrestrial (solar) composition of a given element. While small effects close to the resolution of mass spectrometric techniques can have ambiguous origins, the discovery of large isotopic anomalies in inclusions and grains from primitive meteorites suggests that material from distinct sites of stellar nucleosynthesis has been preserved. Refractory inclusions, which are predominantly composed of the refractory oxides of Al, Ca, Ti, and Mg, in chondritic meteorites commonly have excesses in the heaviest isotopes of Ca, Ti, and Cr which are inferred to have been produced in a supernova. Refractory inclusions also contain excess 26Mg from short lived 26Al decay. However, despite the isotopic anomalies indicating the preservation of distinct nucleosynthetic sites, refractory inclusions have been processed in the solar system and are not interstellar grains. Carbon (graphite and diamond) and silicon carbide grains from the same meteorites also have large isotopic anomalies but these phases are not stable in the oxidized solar nebula which suggests that they are presolar and formed in the circumstellar atmospheres of carbon-rich stars. Diamond has a characteristic signature enriched in the lightest and heaviest isotopes of Xe, and graphite shows a wide range in C isotopic compositions. SiC commonly has C and N isotopic signatures which are characteristic of H-burning in the C-N-O cycle in low-mass stars. Heavier elements such as Si, Ti, Xe, Ba, and Nd, carry an isotopic signature of the s-process. A minor population of SiC (known as Grains X, ca. 1%) are distinct in having decay products of short lived isotopes 26Al (now 26Mg), 44Ti (now 44Ca), and 49V (now 49Ti), as well as 28Si excesses which are characteristic of supernova nucleosynthesis. The preservation of these isotopic anomalies allows the examination of detailed nucleosynthetic pathways in stars. PMID

  5. Review of uranium bioassay techniques

    SciTech Connect

    Bogard, J.S.

    1996-04-01

    A variety of analytical techniques is available for evaluating uranium in excreta and tissues at levels appropriate for occupational exposure control and evaluation. A few (fluorometry, kinetic phosphorescence analysis, {alpha}-particle spectrometry, neutron irradiation techniques, and inductively-coupled plasma mass spectrometry) have also been demonstrated as capable of determining uranium in these materials at levels comparable to those which occur naturally. Sample preparation requirements and isotopic sensitivities vary widely among these techniques and should be considered carefully when choosing a method. This report discusses analytical techniques used for evaluating uranium in biological matrices (primarily urine) and limits of detection reported in the literature. No cost comparison is attempted, although references are cited which address cost. Techniques discussed include: {alpha}-particle spectrometry; liquid scintillation spectrometry, fluorometry, phosphorometry, neutron activation analysis, fission-track counting, UV-visible absorption spectrophotometry, resonance ionization mass spectrometry, and inductively-coupled plasma mass spectrometry. A summary table of reported limits of detection and of the more important experimental conditions associated with these reported limits is also provided.

  6. Uranium industry annual 1994

    SciTech Connect

    1995-07-05

    The Uranium Industry Annual 1994 (UIA 1994) provides current statistical data on the US uranium industry`s activities relating to uranium raw materials and uranium marketing during that survey year. The UIA 1994 is prepared for use by the Congress, Federal and State agencies, the uranium and nuclear electric utility industries, and the public. It contains data for the 10-year period 1985 through 1994 as collected on the Form EIA-858, ``Uranium Industry Annual Survey.`` Data collected on the ``Uranium Industry Annual Survey`` (UIAS) provide a comprehensive statistical characterization of the industry`s activities for the survey year and also include some information about industry`s plans and commitments for the near-term future. Where aggregate data are presented in the UIA 1994, care has been taken to protect the confidentiality of company-specific information while still conveying accurate and complete statistical data. A feature article, ``Comparison of Uranium Mill Tailings Reclamation in the United States and Canada,`` is included in the UIA 1994. Data on uranium raw materials activities including exploration activities and expenditures, EIA-estimated resources and reserves, mine production of uranium, production of uranium concentrate, and industry employment are presented in Chapter 1. Data on uranium marketing activities, including purchases of uranium and enrichment services, and uranium inventories, enrichment feed deliveries (actual and projected), and unfilled market requirements are shown in Chapter 2.

  7. Uranium industry annual 1998

    SciTech Connect

    1999-04-22

    The Uranium Industry Annual 1998 (UIA 1998) provides current statistical data on the US uranium industry`s activities relating to uranium raw materials and uranium marketing. It contains data for the period 1989 through 2008 as collected on the Form EIA-858, ``Uranium Industry Annual Survey.`` Data provides a comprehensive statistical characterization of the industry`s activities for the survey year and also include some information about industry`s plans and commitments for the near-term future. Data on uranium raw materials activities for 1989 through 1998, including exploration activities and expenditures, EIA-estimated reserves, mine production of uranium, production of uranium concentrate, and industry employment, are presented in Chapter 1. Data on uranium marketing activities for 1994 through 2008, including purchases of uranium and enrichment services, enrichment feed deliveries, uranium fuel assemblies, filled and unfilled market requirements, and uranium inventories, are shown in Chapter 2. The methodology used in the 1998 survey, including data edit and analysis, is described in Appendix A. The methodologies for estimation of resources and reserves are described in Appendix B. A list of respondents to the ``Uranium Industry Annual Survey`` is provided in Appendix C. The Form EIA-858 ``Uranium Industry Annual Survey`` is shown in Appendix D. For the readers convenience, metric versions of selected tables from Chapters 1 and 2 are presented in Appendix E along with the standard conversion factors used. A glossary of technical terms is at the end of the report. 24 figs., 56 tabs.

  8. Uranium Oxide Aerosol Transport in Porous Graphite

    SciTech Connect

    Blanchard, Jeremy; Gerlach, David C.; Scheele, Randall D.; Stewart, Mark L.; Reid, Bruce D.; Gauglitz, Phillip A.; Bagaasen, Larry M.; Brown, Charles C.; Iovin, Cristian; Delegard, Calvin H.; Zelenyuk, Alla; Buck, Edgar C.; Riley, Brian J.; Burns, Carolyn A.

    2012-01-23

    The objective of this paper is to investigate the transport of uranium oxide particles that may be present in carbon dioxide (CO2) gas coolant, into the graphite blocks of gas-cooled, graphite moderated reactors. The transport of uranium oxide in the coolant system, and subsequent deposition of this material in the graphite, of such reactors is of interest because it has the potential to influence the application of the Graphite Isotope Ratio Method (GIRM). The GIRM is a technology that has been developed to validate the declared operation of graphite moderated reactors. GIRM exploits isotopic ratio changes that occur in the impurity elements present in the graphite to infer cumulative exposure and hence the reactor’s lifetime cumulative plutonium production. Reference Gesh, et. al., for a more complete discussion on the GIRM technology.

  9. Paragenesis and Geochronology of the Nopal I Uranium Deposit, Mexico

    SciTech Connect

    M. Fayek; M. Ren

    2007-02-14

    Uranium deposits can, by analogy, provide important information on the long-term performance of radioactive waste forms and radioactive waste repositories. Their complex mineralogy and variable elemental and isotopic compositions can provide important information, provided that analyses are obtained on the scale of several micrometers. Here, we present a structural model of the Nopal I deposit as well as petrography at the nanoscale coupled with preliminary U-Th-Pb ages and O isotopic compositions of uranium-rich minerals obtained by Secondary Ion Mass Spectrometry (SIMS). This multi-technique approach promises to provide ''natural system'' data on the corrosion rate of uraninite, the natural analogue of spent nuclear fuel.

  10. The Roots of Minority Giving.

    ERIC Educational Resources Information Center

    Abbe, M. Ann

    2000-01-01

    Discussion of ways to increase minority giving to colleges and universities debunks the myth of "minorities don't give," and reports a recent study of minority philanthropy, which details philanthropic characteristics of four minority cultures: blacks, Hispanics, Asian Americans, and American Indians. Specific strategies recommended include…

  11. Process for electroslag refining of uranium and uranium alloys

    DOEpatents

    Lewis, P.S. Jr.; Agee, W.A.; Bullock, J.S. IV; Condon, J.B.

    1975-07-22

    A process is described for electroslag refining of uranium and uranium alloys wherein molten uranium and uranium alloys are melted in a molten layer of a fluoride slag containing up to about 8 weight percent calcium metal. The calcium metal reduces oxides in the uranium and uranium alloys to provide them with an oxygen content of less than 100 parts per million. (auth)

  12. URANIUM RECOVERY PROCESS

    DOEpatents

    Bailes, R.H.; Long, R.S.; Olson, R.S.; Kerlinger, H.O.

    1959-02-10

    A method is described for recovering uranium values from uranium bearing phosphate solutions such as are encountered in the manufacture of phosphate fertilizers. The solution is first treated with a reducing agent to obtain all the uranium in the tetravalent state. Following this reduction, the solution is treated to co-precipitate the rcduced uranium as a fluoride, together with other insoluble fluorides, thereby accomplishing a substantially complete recovery of even trace amounts of uranium from the phosphate solution. This precipitate usually takes the form of a complex fluoride precipitate, and after appropriate pre-treatment, the uranium fluorides are leached from this precipitate and rccovered from the leach solution.

  13. PRODUCTION OF PURIFIED URANIUM

    DOEpatents

    Burris, L. Jr.; Knighton, J.B.; Feder, H.M.

    1960-01-26

    A pyrometallurgical method for processing nuclear reactor fuel elements containing uranium and fission products and for reducing uranium compound; to metallic uranium is reported. If the material proccssed is essentially metallic uranium, it is dissolved in zinc, the sulution is cooled to crystallize UZn/sub 9/ , and the UZn/sub 9/ is distilled to obtain uranium free of fission products. If the material processed is a uranium compound, the sollvent is an alloy of zinc and magnesium and the remaining steps are the same.

  14. Nurturing the Innovative Minority

    ERIC Educational Resources Information Center

    Gallagher, James J.

    2005-01-01

    This article discusses the innovative minority. Gifted students differ from the average students. There are those who argue that the differences are a matter merely of quantitative degree reference studies of IQ scores, or SAT scores, which are clearly quantitative scales, and point out that gifted students appear at the top level of these scales…

  15. Alcoholism and Minority Populations.

    ERIC Educational Resources Information Center

    Watts, Thomas D.; Wright, Roosevelt, Jr.

    1991-01-01

    Briefly discusses some aspects of the role of the state and the position of minorities in respect to alcoholism policies and services. Includes case study of a Black alcoholic. Refers readers to studies on Black alcoholism, Native American alcoholism, Hispanic alcoholism, and Asian-American alcoholism. (Author/NB)

  16. Minority Student Retention.

    ERIC Educational Resources Information Center

    Henderson, James C.

    1991-01-01

    Discusses the community college's role in Native American education. Describes recruitment, counseling, assessment, remedial, and outreach programs developed by San Juan College to help minority students succeed, and specifically help Native Americans bridge the worlds of public school, reservation, and university. Identifies keys to the programs'…

  17. Positions of minor planets

    NASA Astrophysics Data System (ADS)

    Gressmann, M.

    A continuation of Gressman's (1980) observations is given using the Schmidt-camera 34/40 cm, f = 76. Topocentric positions of several minor planets are presented, and reference stars are obtained from the AGK(3), and applied to the two-star method to avoid any major errors. Parallax constants are also given, along with coordinates for the epoch 1950.0.

  18. Spotlight on Minority Students

    ERIC Educational Resources Information Center

    Yous, Phakdey Chea; Mahamed, Hodman; Kost, Kimberly

    2009-01-01

    This article spotlights minority students in school psychology training programs. Three students from underrepresented backgrounds were asked to reflect on what aspects of their program made them feel welcome and supported. In their discussions, they took the task a step further and furnished ideas about ways in which school psychology training…

  19. Psychological Tests and Minorities.

    ERIC Educational Resources Information Center

    Wright, Brenda Johnson; Isenstein, Vivian R.

    The problems with traditional testing, particularly as they relate to minorities, are discussed; and psychological tests designed specifically for Blacks are reviewed. Considered are general problems, problems with testing at the higher education level and for employment, and moral and legal implications of the testing controversy. The rationale…

  20. Language, Literacy, and Minorities.

    ERIC Educational Resources Information Center

    Skutnabb-Kangas, Tove

    The ideal of a world where bilingualism or multilingualism is a normal and accepted feature is promoted in a commissioned report for International Literacy Year. It is noted that many minority groups are forced into bilingualism as a necessity for survival, but that those skills are rarely seen as an advantage and often seen as a cause of…

  1. PATTERNS OF MINORITY RELATIONS.

    ERIC Educational Resources Information Center

    DUSTER, TROY S.; MACK, RAYMOND W.

    ACCORDING TO SOCIAL SCIENTISTS AND BIOLOGISTS, ALL RACES ARE EQUAL IN ABILITY, NEVERTHELESS, RACIAL DISCRIMINATION EXISTS WHEN THE CULTURE OF A SOCIETY ALLOWS PEOPLE TO EXPRESS THEIR AGRESSIONS IN A SOCIALLY ACCEPTABLE WAY. ONE WAY TO DEFINE GROUP BOUNDARIES IS TO SINGLE OUT A CHARACTERISTIC OF A MINORITY GROUP AND TO INSTITUTIONALIZE THIS…

  2. The Mountaineer Minority

    ERIC Educational Resources Information Center

    Egerton, John; Gaillard, Frye

    1974-01-01

    Discusses the new Appalachian movement, based on the assumption that mountain people are a distinct and maligned cultural minority; the people of Appalachia, white, black and red, have begun to strike back against the dam-builders, strip-miners, and others they say are gouging out the region's mineral resources by the cheapest means possible no…

  3. The Year Ahead: Minorities.

    ERIC Educational Resources Information Center

    Jaschik, Scott

    1987-01-01

    The college outlook is grim for blacks 25 years after James Meredith became the first black to enroll at the University of Mississippi. Both Hispanics and Asian-Americans are misunderstood by college officials, and too little attention has been focused on community colleges, the institutions that serve the most minority students. (MLW)

  4. Assessing Minority Group Children.

    ERIC Educational Resources Information Center

    Phillips, Beeman N., Ed.

    Contents of this book include the following collection of articles: "Assessing Minority Group Children: Challenges for School Psychologists," Thomas Oakland; "The NEA Testing Moratorium," Boyd Bosma; "Cultural Myopia: The Need for a Corrective Lens," Martin H. Gerry; "Assumptions Underlying Psychological Testing," T. Ernest Newland;…

  5. Isotopically Modified Molybdenum: Production for Application in Nuclear Energy

    NASA Astrophysics Data System (ADS)

    Smirnov, A. Yu.; Bonarev, A. K.; Sulaberidze, G. A.; Borisevich, V. D.; Kulikov, G. G.; Shmelev, A. N.

    The possibility to use the isotopically modified molybdenum as a constructive material for the fuel rods of light water and fast reactors is discussed. The calculations demonstrate that the isotopically modified molybdenum with an average neutron absorption cross-section comparable to that of zirconium can be obtained with the reasonable for practice cost by a cascade of gas centrifuges, specially designed for separation of non-uranium isotopes.

  6. Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico

    SciTech Connect

    Goldstein, S.J.; Abdel-Fattah, A.I.; Murrell, M.T.; Dobson, P.F.; Norman, D.E.; Amato, R.S.; Nunn, A. J.

    2009-10-01

    Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ({approx}10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that {sup 230}Th/{sup 238}U activity ratios range from 0.005-0.48 and {sup 226}Ra/{sup 238}U activity ratios range from 0.006-113. {sup 239}Pu/{sup 238}U mass ratios for the saturated zone are <2 x 10{sup -14}, and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order {sup 238}U{approx}{sup 226}Ra > {sup 230}Th{approx}{sup 239}Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

  7. Uranium-series constraints on radionuclide transport and groundwater flow at the Nopal I uranium deposit, Sierra Pena Blanca, Mexico.

    PubMed

    Goldstein, Steven J; Abdel-Fattah, Amr I; Murrell, Michael T; Dobson, Patrick F; Norman, Deborah E; Amato, Ronald S; Nunn, Andrew J

    2010-03-01

    Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low ( approximately 10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that (230)Th/(238)U activity ratios range from 0.005 to 0.48 and (226)Ra/(238)U activity ratios range from 0.006 to 113. (239)Pu/(238)U mass ratios for the saturated zone are <2 x 10(-14), and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order (238)U approximately (226)Ra > (230)Th approximately (239)Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit. PMID:20136119

  8. NICKEL COATED URANIUM ARTICLE

    DOEpatents

    Gray, A.G.

    1958-10-01

    Nickel coatings on uranium and various methods of obtaining such coatings are described. Specifically disclosed are such nickel or nickel alloy layers as barriers between uranium and aluminum- silicon, chromium, or copper coatings.

  9. METHOD FOR PURIFYING URANIUM

    DOEpatents

    Knighton, J.B.; Feder, H.M.

    1960-04-26

    A process is given for purifying a uranium-base nuclear material. The nuclear material is dissolved in zinc or a zinc-magnesium alloy and the concentration of magnesium is increased until uranium precipitates.

  10. DEPLETED URANIUM TECHNICAL WORK

    EPA Science Inventory

    The Depleted Uranium Technical Work is designed to convey available information and knowledge about depleted uranium to EPA Remedial Project Managers, On-Scene Coordinators, contractors, and other Agency managers involved with the remediation of sites contaminated with this mater...

  11. Uranium from phosphate ores

    SciTech Connect

    Hurst, F.J.

    1983-01-01

    The following topics are described briefly: the way phosphate fertilizers are made; how uranium is recovered in the phosphate industry; and how to detect covert uranium recovery operations in a phsophate plant.

  12. Uranium-Series Constraints on Subrepository Water Flow at Yucca Mountain, Nevada

    SciTech Connect

    L.A. Neymark; J.B. Paces; S.J. Chipera; D.T. Vaniman

    2006-03-10

    Mineral abundances and whole-rock chemical and uranium-series isotopic compositions were measured in unfractured and rubble core samples from borehole USWSD-9 in the same layers of variably zeolitized tuffs that underlie the proposed nuclear waste repository at Yucca Mountain, Nevada. Uranium concentrations and isotopic compositions also were measured in pore water from core samples from the same rock units and rock leachates representing loosely bound U adsorbed on mineral surfaces or contained in readily soluble secondary minerals. The chemical and isotopic data were used to evaluate differences in water-rock interaction between fractured and unfractured rock and between fracture surfaces and rock matrix. Samples of unfractured and rubble fragments (about 1 centimeter) core and material from fracture surfaces show similar amounts of uranium-series disequilibrium, recording a complex history of sorption and loss of uranium over the past 1 million years. The data indicate that fractures in zeolitized tuffs may not have had greater amounts of water-rock interaction than the rock matrix. The data also show that rock matrix from subrepository units is capable of scavenging uranium with elevated uranium-234/uranium-238 from percolating water and that retardation of radionuclides and dose reduction may be greater than currently credited to this aspect of the natural barrier. Uranium concentrations of pore water and the rock leachates are used to estimate long-term in situ uranium partition coefficient values greater than 7 milliliters per gram.

  13. Depleted uranium analysis in blood by inductively coupled plasma mass spectrometry

    USGS Publications Warehouse

    Todorov, T.I.; Xu, H.; Ejnik, J.W.; Mullick, F.G.; Squibb, K.; McDiarmid, M.A.; Centeno, J.A.

    2009-01-01

    In this study we report depleted uranium (DU) analysis in whole blood samples. Internal exposure to DU causes increased uranium levels as well as change in the uranium isotopic composition in blood specimen. For identification of DU exposure we used the 235U/238U ratio in blood samples, which ranges from 0.00725 for natural uranium to 0.002 for depleted uranium. Uranium quantification and isotopic composition analysis were performed by inductively coupled plasma mass spectrometry. For method validation we used eight spiked blood samples with known uranium concentrations and isotopic composition. The detection limit for quantification was determined to be 4 ng L-1 uranium in whole blood. The data reproduced within 1-5% RSD and an accuracy of 1-4%. In order to achieve a 235U/238U ratio range of 0.00698-0.00752% with 99.7% confidence limit a minimum whole blood uranium concentration of 60 ng L??1 was required. An additional 10 samples from a cohort of veterans exposed to DU in Gulf War I were analyzed with no knowledge of their medical history. The measured 235U/ 238U ratios in the blood samples were used to identify the presence or absence of DU exposure within this patient group. ?? 2009 The Royal Society of Chemistry.

  14. Uranium industry annual 1995

    SciTech Connect

    1996-05-01

    The Uranium Industry Annual 1995 (UIA 1995) provides current statistical data on the U.S. uranium industry`s activities relating to uranium raw materials and uranium marketing. The UIA 1995 is prepared for use by the Congress, Federal and State agencies, the uranium and nuclear electric utility industries, and the public. It contains data for the period 1986 through 2005 as collected on the Form EIA-858, ``Uranium Industry Annual Survey``. Data collected on the ``Uranium Industry Annual Survey`` provide a comprehensive statistical characterization of the industry`s plans and commitments for the near-term future. Where aggregate data are presented in the UIA 1995, care has been taken to protect the confidentiality of company-specific information while still conveying accurate and complete statistical data. Data on uranium raw materials activities for 1986 through 1995 including exploration activities and expenditures, EIA-estimated reserves, mine production of uranium, production of uranium concentrate, and industry employment are presented in Chapter 1. Data on uranium marketing activities for 1994 through 2005, including purchases of uranium and enrichment services, enrichment feed deliveries, uranium fuel assemblies, filled and unfilled market requirements, uranium imports and exports, and uranium inventories are shown in Chapter 2. The methodology used in the 1995 survey, including data edit and analysis, is described in Appendix A. The methodologies for estimation of resources and reserves are described in Appendix B. A list of respondents to the ``Uranium Industry Annual Survey`` is provided in Appendix C. For the reader`s convenience, metric versions of selected tables from Chapters 1 and 2 are presented in Appendix D along with the standard conversion factors used. A glossary of technical terms is at the end of the report. 14 figs., 56 tabs.

  15. PREPARATION OF URANIUM HEXAFLUORIDE

    DOEpatents

    Lawroski, S.; Jonke, A.A.; Steunenberg, R.K.

    1959-10-01

    A process is described for preparing uranium hexafluoride from carbonate- leach uranium ore concentrate. The briquetted, crushed, and screened concentrate is reacted with hydrogen fluoride in a fluidized bed, and the uranium tetrafluoride formed is mixed with a solid diluent, such as calcium fluoride. This mixture is fluorinated with fluorine and an inert diluent gas, also in a fluidized bed, and the uranium hexafluoride obtained is finally purified by fractional distillation.

  16. PROCESS OF PURIFYING URANIUM

    DOEpatents

    Seaborg, G.T.; Orlemann, E.F.; Jensen, L.H.

    1958-12-23

    A method of obtaining substantially pure uranium from a uranium composition contaminated with light element impurities such as sodium, magnesium, beryllium, and the like is described. An acidic aqueous solution containing tetravalent uranium is treated with a soluble molybdate to form insoluble uranous molybdate which is removed. This material after washing is dissolved in concentrated nitric acid to obtaln a uranyl nitrate solution from which highly purified uranium is obtained by extraction with ether.

  17. PRODUCTION OF URANIUM TETRAFLUORIDE

    DOEpatents

    Shaw, W.E.; Spenceley, R.M.; Teetzel, F.M.

    1959-08-01

    A method is presented for producing uranium tetrafluoride from the gaseous hexafluoride by feeding the hexafluoride into a high temperature zone obtained by the recombination of molecularly dissociated hydrogen. The molal ratio of hydrogen to uranium hexnfluoride is preferably about 3 to 1. Uranium tetrafluoride is obtained in a finely divided, anhydrous state.

  18. Isotopic signatures by bulk analyses

    SciTech Connect

    Efurd, D.W.; Rokop, D.J.

    1997-12-01

    Los Alamos National Laboratory has developed a series of measurement techniques for identification of nuclear signatures by analyzing bulk samples. Two specific applications for isotopic fingerprinting to identify the origin of anthropogenic radioactivity in bulk samples are presented. The first example is the analyses of environmental samples collected in the US Arctic to determine the impact of dumping of radionuclides in this polar region. Analyses of sediment and biota samples indicate that for the areas sampled the anthropogenic radionuclide content of sediments was predominantly the result of the deposition of global fallout. The anthropogenic radionuclide concentrations in fish, birds and mammals were very low. It can be surmised that marine food chains are presently not significantly affected. The second example is isotopic fingerprinting of water and sediment samples from the Rocky Flats Facility (RFP). The largest source of anthropogenic radioactivity presently affecting surface-waters at RFP is the sediments that are currently residing in the holding ponds. One gram of sediment from a holding pond contains approximately 50 times more plutonium than 1 liter of water from the pond. Essentially 100% of the uranium in Ponds A-1 and A-2 originated as depleted uranium. The largest source of radioactivity in the terminal Ponds A-4, B-5 and C-2 was naturally occurring uranium and its decay product radium. The uranium concentrations in the waters collected from the terminal ponds contained 0.05% or less of the interim standard calculated derived concentration guide for uranium in waters available to the public. All of the radioactivity observed in soil, sediment and water samples collected at RFP was naturally occurring, the result of processes at RFP or the result of global fallout. No extraneous anthropogenic alpha, beta or gamma activities were detected. The plutonium concentrations in Pond C-2 appear to vary seasonally.

  19. Tags to Track Illicit Uranium and Plutonium

    SciTech Connect

    Haire, M. Jonathan; Forsberg, Charles W.

    2007-07-01

    With the expansion of nuclear power, it is essential to avoid nuclear materials from falling into the hands of rogue nations, terrorists, and other opportunists. This paper examines the idea of detection and attribution tags for nuclear materials. For a detection tag, it is proposed to add small amounts [about one part per billion (ppb)] of {sup 232}U to enriched uranium to brighten its radioactive signature. Enriched uranium would then be as detectable as plutonium and thus increase the likelihood of intercepting illicit enriched uranium. The use of rare earth oxide elements is proposed as a new type of 'attribution' tag for uranium and thorium from mills, uranium and plutonium fuels, and other nuclear materials. Rare earth oxides are chosen because they are chemically compatible with the fuel cycle, can survive high-temperature processing operations in fuel fabrication, and can be chosen to have minimal neutronic impact within the nuclear reactor core. The mixture of rare earths and/or rare earth isotopes provides a unique 'bar code' for each tag. If illicit nuclear materials are recovered, the attribution tag can identify the source and lot of nuclear material, and thus help police reduce the possible number of suspects in the diversion of nuclear materials based on who had access. (authors)

  20. Minor planet databases

    NASA Astrophysics Data System (ADS)

    Rykhlova, L.; Bakanas, E.

    We cast a retrospective look at the mankind's acquaintance with minor bodies of the Solar System, at the explosive growth in their discoveries resulting from the technological progress, and at gradual understanding of the danger to our very existence that some of them might actually pose. Then, we review current effort, of the astronomical community in general and of its Russian part in particular, to integrate our rapidly expanding knowledge of the potential Earth impactors and to make it readily available online.

  1. Isotope separation

    DOEpatents

    Bartlett, Rodney J.; Morrey, John R.

    1978-01-01

    A method and apparatus is described for separating gas molecules containing one isotope of an element from gas molecules containing other isotopes of the same element in which all of the molecules of the gas are at the same electronic state in their ground state. Gas molecules in a gas stream containing one of the isotopes are selectively excited to a different electronic state while leaving the other gas molecules in their original ground state. Gas molecules containing one of the isotopes are then deflected from the other gas molecules in the stream and thus physically separated.

  2. Disproportionate minority contact.

    PubMed

    Piquero, Alex R

    2008-01-01

    For many years, notes Alex Piquero, youth of color have been overrepresented at every stage of the U.S. juvenile justice system. As with racial disparities in a wide variety of social indicators, the causes of these disparities are not immediately apparent. Some analysts attribute the disparities to "differential involvement"--that is, to differences in offending by minorities and whites. Others attribute them to "differential selection"--that is, to the fact that the justice system treats minority and white offenders in different ways. Still others believe the explanation lies in a combination of the two. Differential involvement may be important earlier in the judicial process, especially in youths' contacts with police, and may influence differential selection later as individuals make their way through the juvenile justice system. Adjudicating between these options, says Piquero, is difficult and may even be impossible. Asking how much minority overrepresentation is due to differences in offending and how much to differences in processing no longer seems a helpful way to frame the discussion. Piquero urges future research to move beyond the debate over "which one matters more" and seek to understand how each of the two hypotheses can explain both the fact of minority overrepresentation in the juvenile justice system and how best to address it. Piquero cites many sizable gaps in the research and policy-relevant literature. Work is needed especially, he says, in analyzing the first stage of the justice system that juveniles confront: police contacts. The police are a critical part of the juvenile justice decision-making system and are afforded far more discretion than any other formal agent of social control, but researchers have paid surprisingly little attention to contacts between police and citizens, especially juveniles. Piquero notes that some states and localities are undertaking initiatives to reduce racial and ethnic disparities. He urges researchers and

  3. The Effectiveness of Minority Teachers on Minority Student Success.

    ERIC Educational Resources Information Center

    Salinas, Jose P.

    This paper examines the shortage of minority teachers and explores the high priority that exists among parents, teachers, and the business community to work toward a diversified teaching force, focusing on the U.S. Hispanic population and investigating whether minority teachers in the classroom can result in minority student success in school. The…

  4. URANIUM SEPARATION PROCESS

    DOEpatents

    Hyde, E.K.; Katzin, L.I.; Wolf, M.J.

    1959-07-14

    The separation of uranium from a mixture of uranium and thorium by organic solvent extraction from an aqueous solution is described. The uranium is separrted from an aqueous mixture of uranium and thorium nitrates 3 N in nitric acid and containing salting out agents such as ammonium nitrate, so as to bring ihe total nitrate ion concentration to a maximum of about 8 N by contacting the mixture with an immiscible aliphatic oxygen containing organic solvent such as diethyl carbinol, hexone, n-amyl acetate and the like. The uranium values may be recovered from the organic phase by back extraction with water.

  5. PRODUCTION OF URANIUM

    DOEpatents

    Spedding, F.H.; Wilhelm, H.A.; Keller, W.H.

    1958-04-15

    The production of uranium metal by the reduction of uranium tetrafluoride is described. Massive uranium metal of high purily is produced by reacting uranium tetrafluoride with 2 to 20% stoichiometric excess of magnesium at a temperature sufficient to promote the reaction and then mantaining the reaction mass in a sealed vessel at temperature in the range of 1150 to 2000 d C, under a superatomospheric pressure of magnesium for a period of time sufficient 10 allow separation of liquid uranium and liquid magnesium fluoride into separate layers.

  6. PROCESS OF RECOVERING URANIUM

    DOEpatents

    Carter, J.M.; Larson, C.E.

    1958-10-01

    A process is presented for recovering uranium values from calutron deposits. The process consists in treating such deposits to produce an oxidlzed acidic solution containing uranium together with the following imparities: Cu, Fe, Cr, Ni, Mn, Zn. The uranium is recovered from such an impurity-bearing solution by adjusting the pH of the solution to the range 1.5 to 3.0 and then treating the solution with hydrogen peroxide. This results in the precipitation of uranium peroxide which is substantially free of the metal impurities in the solution. The peroxide precipitate is then separated from the solution, washed, and calcined to produce uranium trioxide.

  7. URANIUM RECOVERY PROCESS

    DOEpatents

    Yeager, J.H.

    1958-08-12

    In the prior art processing of uranium ores, the ore is flrst digested with nitric acid and filtered, and the uranium values are then extracted tom the filtrate by contacting with an organic solvent. The insoluble residue has been processed separately in order to recover any uranium which it might contain. The improvement consists in contacting a slurry, composed of both solution and residue, with the organic solvent prior to filtration. Tbe result is that uranium values contained in the residue are extracted along with the uranium values contained th the solution in one step.

  8. Tetravalent uranium in calcite.

    SciTech Connect

    Sturchio, N. C.; Antonio, M. R.; Soderholm, L.; Sutton, S. R.; Brannon, J. C.; Univ. of Chicago; Washington Univ.

    1998-08-14

    X-ray absorption spectroscopy and x-ray fluorescence microprobe studies of 35-million-year-old calcite from a Mississippi Valley-type zinc ore deposit indicate substitution of tetravalent uranium for divalent calcium. Thus, tetravalent uranium has a stable location in calcite deposited under reducing conditions. This result validates uranium-series dating methods (including uranium/lead dating) for ancient calcite and shows that calcite provides a sink for uranium in deep groundwater aquifers and anoxic lacustrine and marine basins.

  9. Tetravalent uranium in calcite

    PubMed

    Sturchio; Antonio; Soderholm; Sutton; Brannon

    1998-08-14

    X-ray absorption spectroscopy and x-ray fluorescence microprobe studies of 35-million-year-old calcite from a Mississippi Valley-type zinc ore deposit indicate substitution of tetravalent uranium for divalent calcium. Thus, tetravalent uranium has a stable location in calcite deposited under reducing conditions. This result validates uranium-series dating methods (including uranium/lead dating) for ancient calcite and shows that calcite provides a sink for uranium in deep groundwater aquifers and anoxic lacustrine and marine basins. PMID:9703507

  10. Minority Health and Health Disparities

    MedlinePlus

    ... Minority Health and Health Disparities Certain ethnic and racial minorities as well as other underserved populations experience ... disorders than do non-Hispanic whites, ethnic and racial disparities still exist for alcohol-related diseases, problems, ...

  11. Method for converting uranium oxides to uranium metal

    DOEpatents

    Duerksen, Walter K.

    1988-01-01

    A process is described for converting scrap and waste uranium oxide to uranium metal. The uranium oxide is sequentially reduced with a suitable reducing agent to a mixture of uranium metal and oxide products. The uranium metal is then converted to uranium hydride and the uranium hydride-containing mixture is then cooled to a temperature less than -100.degree. C. in an inert liquid which renders the uranium hydride ferromagnetic. The uranium hydride is then magnetically separated from the cooled mixture. The separated uranium hydride is readily converted to uranium metal by heating in an inert atmosphere. This process is environmentally acceptable and eliminates the use of hydrogen fluoride as well as the explosive conditions encountered in the previously employed bomb-reduction processes utilized for converting uranium oxides to uranium metal.

  12. 78 FR 17942 - Request To Amend a License To Export High-Enriched Uranium

    Federal Register 2010, 2011, 2012, 2013, 2014

    2013-03-25

    ... promulgated in August 2007, 72 FR 49139 (Aug. 28, 2007). Information about filing electronically is available... medical isotope March 11, 2013 uranium) the list of production at the XSNM3622/02 research reactor... fuel or targets for medical isotope production Dated this 14th day of March 2013 at Rockville,...

  13. A Graphical Examination of Uranium and Plutonium Fissility

    ERIC Educational Resources Information Center

    Reed, B. Cameron

    2008-01-01

    The issue of why only particular isotopes of uranium and plutonium are suitable for use in nuclear weapons is analyzed with the aid of graphs and semiquantitative discussions of parameters such as excitation energies, fission barriers, reaction cross-sections, and the role of processes such as [alpha]-decay and spontaneous fission. The goal is to…

  14. 31 CFR 540.317 - Uranium feed; natural uranium feed.

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 31 Money and Finance:Treasury 3 2014-07-01 2014-07-01 false Uranium feed; natural uranium feed... (Continued) OFFICE OF FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed....

  15. 31 CFR 540.317 - Uranium feed; natural uranium feed.

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 31 Money and Finance:Treasury 3 2013-07-01 2013-07-01 false Uranium feed; natural uranium feed... (Continued) OFFICE OF FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed....

  16. 31 CFR 540.317 - Uranium feed; natural uranium feed.

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 31 Money and Finance:Treasury 3 2012-07-01 2012-07-01 false Uranium feed; natural uranium feed... (Continued) OFFICE OF FOREIGN ASSETS CONTROL, DEPARTMENT OF THE TREASURY HIGHLY ENRICHED URANIUM (HEU) AGREEMENT ASSETS CONTROL REGULATIONS General Definitions § 540.317 Uranium feed; natural uranium feed....

  17. Career Education: Implications for Minorities.

    ERIC Educational Resources Information Center

    Sheppard, N. Alan; Witherspoon, Everette L.

    In general, minorities, especially blacks, approach career education warily, fearing it might turn out to be a new name for an old game. Statistics indicate the minority dilemma; for example, unemployment among minorities 16 and older is nearly twice the white unemployment rate. A number of critical questions about career education as related to…

  18. Long-term criticality control in radioactive waste disposal facilities using depleted uranium

    SciTech Connect

    Forsberg, C.W.

    1997-02-19

    Plant photosynthesis has created a unique planetary-wide geochemistry - an oxidizing atmosphere with oxidizing surface waters on a planetary body with chemically reducing conditions near or at some distance below the surface. Uranium is four orders of magnitude more soluble under chemically oxidizing conditions than it is under chemically reducing conditions. Thus, uranium tends to leach from surface rock and disposal sites, move with groundwater, and concentrate where chemically reducing conditions appear. Earth`s geochemistry concentrates uranium and can separate uranium from all other elements except oxygen, hydrogen (in water), and silicon (silicates, etc). Fissile isotopes include {sup 235}U, {sup 233}U, and many higher actinides that eventually decay to one of these two uranium isotopes. The potential for nuclear criticality exists if the precipitated uranium from disposal sites has a significant fissile enrichment, mass, and volume. The earth`s geochemistry suggests that isotopic dilution of fissile materials in waste with {sup 238}U is a preferred strategy to prevent long-term nuclear criticality in and beyond the boundaries of waste disposal facilities because the {sup 238}U does not separate from the fissile uranium isotopes. Geological, laboratory, and theoretical data indicate that the potential for nuclear criticality can be minimized by diluting fissile materials with-{sup 238}U to 1 wt % {sup 235}U equivalent.

  19. Calculating Capstone depleted uranium aerosol concentrations from beta activity measurements.

    PubMed

    Szrom, Frances; Falo, Gerald A; Parkhurst, Mary Ann; Whicker, Jeffrey J; Alberth, David P

    2009-03-01

    Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the DU source term for the subsequent Human Health Risk Assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that the equilibrium between the uranium isotopes and their immediate short-lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Values for the equilibrium fraction ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92. This paper describes the process used and adjustments necessary to calculate uranium mass from proportional counting measurements. PMID:19204483

  20. Calculating Capstone Depleted Uranium Aerosol Concentrations from Beta Activity Measurements

    SciTech Connect

    Szrom, Fran; Falo, Gerald A.; Parkhurst, MaryAnn; Whicker, Jeffrey J.; Alberth, David P.

    2009-03-01

    Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the depleted uranium (DU) source term for the subsequent human health risk assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that the equilibrium between the uranium isotopes and their immediate short lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Correction factors for the disrupted equilibrium ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92.