234U— 238U— 230Th— 232Th systematics in saline groundwaters from central Missouri

NASA Astrophysics Data System (ADS)

Banner, Jay L.; Wasserburg, G. J.; Chen, James H.; Moore, Clyde H.

1990-12-01

Saline groundwaters with 4.7 to 26‰ total dissolved solids were sampled from springs and artesian wells in Mississippian and Ordovician carbonates and sandstones in central Missouri. U—Th isotopic variations provide a means of evaluating processes of water-rock interaction and fluid mixing and estimating the time scales of element transport. Recently developed mass spectrometric techniques are used to make isotopic measurements on small-volume groundwater samples (0.1-4 l) with high precision (e.g., < ±5% for 234U/ 238U activity ratios). The groundwaters have a wide range of 238U concentrations, 50 × 10 -12 to 200 × 10 -12 g/g; 234U/ 234U activity ratios, 2.15-16.0; 232Th concentrations, 0.10 × 10 -12 to 33 × 10 -12 g/g; and 230Th concentrations, 0.91 × 10 -17 to 26 × 10 -17 g/g. Unfiltered and filtered (0.4 μm, 0.1 μm) aliquots of a saline sample have the same isotopic composition and concentration of U, indicating that 234U and 238U occur almost entirely as dissolved species. The concentration of 232Th is up to seven times lower in filtered vs. unfiltered aliquots, indicating that 232Th is predominantly associated with particulates in the groundwaters. In contrast, most of the 230Th is in solution. Previous geochemical studies indicate that: (1) the saline waters originated as meteoric recharge and evolved through halite dissolution, reactions with silicates and saline-dilute mixing processes during a long-distance flow history; and (2) interaction with limestone and dolomite aquifer rocks in central Missouri has been limited. A consistent relationship between U/Ca and 234U/ 238U activity ratio is observed in the groundwaters and provides constraints on the U/Ca ratios and 234U/ 238U activity ratios of end-member reservoirs and on the processes of isotopic exchange in this water-rock system. Model calculations that simulate (1) saline-dilute groundwater mixing and (2) limited extents of dissolution of carbonate aquifer minerals by the groundwaters can account for the variations in U/Ca, 234U/ 238U and 18O/ 16O in the suite of water samples. The model calculations demonstrate that dissolved U isotopic compositions can be a sensitive indicator of water-rock interaction, which in turn limits the usefulness of 234U— 238U disequilibria for groundwater age determinations. The concentration of dissolved 230Th in the groundwaters is (1) two to three orders of magnitude below 230Th— 234U equilibrium activity levels, and (2) significantly in excess of concentrations estimated for the supply of Th to solution via desorption and dissolution. A model involving the derivation of the excess 230Th from the in situ decay of dissolved 234U in the groundwaters indicates the operation of an adsorption mechanism on the time scale of 10-10 3 years. The results reported here may have broader application to the assessment and management of hazardous chemical species in natural environments.

Seasonal progression of uranium series isotopes in subglacial meltwater: Implications for subglacial storage time

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arendt, Carli A.; Aciego, Sarah M.; Sims, Kenneth W. W.

The residence time of subglacial meltwater impacts aquifer recharge, nutrient production, and chemical signals that reflect underlying bedrock/substrate, but is inaccessible to direct observation. We report the seasonal evolution of subglacial meltwater chemistry from the 2011 melt season at the terminus of the Athabasca Glacier, Canada. We also measured major and trace analytes and U-series isotopes for twenty-nine bulk meltwater samples collected over the duration of the melt season. This dataset, which is the longest time-series record of ( 234U/ 238U) isotopes in a glacial meltwater system, provides insight into the hydrologic evolution of the subglacial system during active melting.more » Meltwater samples, measured from the outflow, were analyzed for ( 238U), ( 222Rn) and ( 234U/ 238U)activity, conductivity, alkalinity, pH and major cations. Subglacial meltwater varied in [238U] and (222Rn) from 23 to 832 ppt and 9 to 171 pCi/L, respectively. Activity ratios of ( 234U/ 238U) ranged from 1.003 to 1.040, with the highest ( 238U), ( 222Rn) and ( 234U/ 238U)activity values occurring in early May when delayed-flow basal meltwater composed a significant portion of the bulk melt. Furthemore, from the chemical evolution of the meltwater, we posit that the relative subglacial water residence times decrease over the course of the melt season. This decrease in qualitative residence time during active melt is consistent with prior field studies and model-predicted channel switching from a delayed, distributed network to a fast, channelized network flow. As such, our study provides support for linking U-series isotopes to storage lengths of meltwater beneath glacial systems as subglacial hydrologic networks evolve with increased melting and channel network efficiency.« less

Seasonal progression of uranium series isotopes in subglacial meltwater: Implications for subglacial storage time

DOE PAGES

Arendt, Carli A.; Aciego, Sarah M.; Sims, Kenneth W. W.; ...

2017-07-31

The residence time of subglacial meltwater impacts aquifer recharge, nutrient production, and chemical signals that reflect underlying bedrock/substrate, but is inaccessible to direct observation. We report the seasonal evolution of subglacial meltwater chemistry from the 2011 melt season at the terminus of the Athabasca Glacier, Canada. We also measured major and trace analytes and U-series isotopes for twenty-nine bulk meltwater samples collected over the duration of the melt season. This dataset, which is the longest time-series record of ( 234U/ 238U) isotopes in a glacial meltwater system, provides insight into the hydrologic evolution of the subglacial system during active melting.more » Meltwater samples, measured from the outflow, were analyzed for ( 238U), ( 222Rn) and ( 234U/ 238U)activity, conductivity, alkalinity, pH and major cations. Subglacial meltwater varied in [238U] and (222Rn) from 23 to 832 ppt and 9 to 171 pCi/L, respectively. Activity ratios of ( 234U/ 238U) ranged from 1.003 to 1.040, with the highest ( 238U), ( 222Rn) and ( 234U/ 238U)activity values occurring in early May when delayed-flow basal meltwater composed a significant portion of the bulk melt. Furthemore, from the chemical evolution of the meltwater, we posit that the relative subglacial water residence times decrease over the course of the melt season. This decrease in qualitative residence time during active melt is consistent with prior field studies and model-predicted channel switching from a delayed, distributed network to a fast, channelized network flow. As such, our study provides support for linking U-series isotopes to storage lengths of meltwater beneath glacial systems as subglacial hydrologic networks evolve with increased melting and channel network efficiency.« less

234U/238U isotope data from groundwater and solid-phase leachate samples near Tuba City Open Dump, Tuba City, Arizona

USGS Publications Warehouse

Johnson, Raymond H.; Horton, Robert J.; Otton, James K.; Ketterer, Michael K.

2012-01-01

This report releases 234U/238U isotope data, expressed as activity ratios, and uranium concentration data from analyses completed at Northern Arizona University for groundwater and solid-phase leachate samples that were collected in and around Tuba City Open Dump, Tuba City, Arizona, in 2008.

Estimated Marine Residence Times for Drowned Barbadian Paleoreefs

NASA Astrophysics Data System (ADS)

Mey, J. L.

2008-12-01

Fossil corals are used to estimate past sea level and also to calibrate 14C ages with the aid of U-Th and U-Pa dating methods. These coral fossils have often been subaerially exposed and thus are affected by diagenesis during their initial interaction with fresh water. In an effort to understand when such disequilibria in fossil coral reefs occurred, we have quantified our 'dissolution-cum-adsorption' model (Mey, 2008) for the uranium series disequilibria using a geometrical construction, based on the evolution of the activities in a 230Th/238U versus 234U/238U diagram for closed versus open systems. The traditional age equations for the uranium-series with excess daughters have been used to construct a relationship between (i) the angles of the equal age lines in the 230Th/238U versus 234U/238U activity diagrams, and (ii) the quantified angles of the regressed lines of several uranium series disequilibria trends from Barbados. Our results indicate that the severity of the Barbados uranium series disequilibria is not only explained by 234U and 230Th addition, but may also reflect a loss of 238U through dissolution of coral skeletal structure. The net effect is 238U removal, whereas 234U and 230Th remain; thus, the disequilibria for the extant coral increase the excess daughters' ratio. Our results further indicate that the activity of 234U is reduced (compared to 230Th), as would be expected in regard to the lower mobility of trapped 230Th. It is proposed that the major dissolution that caused the uranium series disequilibria occurred during one relatively short-lived event when the paleoreefs experienced the very first freshwater exposure. During this event, the diagenetic potential was at its maximum for redistribution of the uranium series; this then caused the 234U and the 230Th to behave in a systematic way, resulting in linear trends. The linear trends in the open system uranium series were set early, as shown in the 230Th/238U versus 234U/238U activity diagrams. The timing of the first exposure of the freshwater in the reefs is calculated based on the results of our new model. From the relationship between, (i) dissolution, (ii) in-grown 230Th, and (iii) excess 234U, we derived that the 60,000 old Marine Isotope stage 3 (MIS 3) reef was exposed to freshwater 36-38,000 years after growth in the marine environment. We have calculated these 'marine residence times' for the MIS 3 5a, 5c, 5e, 6.0, 7a and 7c reefs; our results correspond with the duration of the sea level high stand in each of the stages. References: Mey, J. L., (2008) The Uranium Series Diagenesis and the Morphology of Drowned Barbadian Paleoreefs, PhD dissertation, 325pp: Graduate Center, City University of New York, New York.

The timing of high sea levels over the past 200,000 years

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gallup, C.D.; Edwards, R.L.; Johnson, R.G.

1994-02-11

The [sup 230]Th ages and [sup 234]U/[sup 238]U ratios were determined for Barbados corals that grew during periods of high sea level within the last 200,000 years. The similarity of the initial [sup 234]U/[sup 238]U ratios of some of the corals to the modern marine value suggests that these samples are pristine and that the marine [sup 234]U/[sup 238]U ratio 83,000 and 200,000 years ago was within 2 per mil of the modern value. The accuracies of the [sup 230]Th ages are evaluated on the basis of the [sup 234]U/[sup 238]U values and a model of the behavior of uraniummore » and thorium isotopes during diagenesis. For the last three interglacial and two intervening interstadial periods, sea level peaked at or after peaks in summer insolation in the Northern Hemisphere. This overall pattern supports the idea that glacial-interglacial cycles are caused by changes in Earth's orbital geometry. The sea-level drop at the end of the penultimate interglacial, the last interglacial, and a subsequent interstadial period lagged behind the decrease in insolation by 5,000 to 10,000 years.« less

206Pb-230Th-234U-238U and 207Pb-235U geochronology of Quaternary opal, Yucca Mountain, Nevada

USGS Publications Warehouse

Neymark, Leonid A.; Amelin, Yuri V.; Paces, James B.

2000-01-01

U–Th–Pb isotopic systems have been studied in submillimeter-thick outermost layers of Quaternary opal occurring in calcite–silica fracture and cavity coatings within Tertiary tuffs at Yucca Mountain, Nevada, USA. These coatings preserve a record of paleohydrologic conditions at this site, which is being evaluated as a potential high-level nuclear waste repository. The opal precipitated from groundwater is variably enriched in 234U (measured 234U/238U activity ratio 1.124–6.179) and has high U (30–313 ppm), low Th (0.008–3.7 ppm), and low common Pb concentrations (measured 206Pb/204Pb up to 11,370). It has been demonstrated that the laboratory acid treatment used in this study to clean sample surfaces and to remove adherent calcite, did not disturb U–Th–Pb isotopic systems in opal. The opal ages calculated from 206Pb∗/238U and 207Pb∗/235U ratios display strong reverse discordance because of excess radiogenic 206Pb∗ derived from the elevated initial 234U. The data are best interpreted using projections of a new four-dimensional concordia diagram defined by 206Pb∗/238U, 207Pb∗/235U, 234U/238Uactivity, and 230Th/238Uactivity. Ages and initial 234U/238U activity ratios have been calculated using different projections of this diagram and tested for concordance. The data are discordant, that is observed 207Pb∗/235U ages of 170 ± 32 (2σ) to 1772 ± 40 ka are systematically older than 230Th/U ages of 34.1 ± 0.6 to 452 ± 32 ka. The age discordance is not a result of migration of uranium and its decay products under the open system conditions, but a consequence of noninstantaneous growth of opal. Combined U–Pb and 230Th/U ages support the model of slow mineral deposition at the rates of millimeters per million years resulting in layering on a scale too fine for mechanical sampling. In this case, U–Pb ages provide more accurate estimates of the average age for mixed multiage samples than 230Th/U ages, because ages based on shorter-lived isotopes are nonlinearly biased by younger mineral additions. Use of the combined U–Th–Pb technique to date Yucca Mountain Quaternary opals significantly extends the age range beyond that of the 230Th/U dating method and shows that selected fracture pathways in the unsaturated zone felsic tuffs of Yucca Mountain have been active throughout the Quaternary.

Radioactivity in three species of eastern Mediterranean jellyfish.

PubMed

Mamish, S; Al-Masri, M S; Durgham, H

2015-11-01

Activity concentrations of (137)Cs, (40)K, (210)Po, (210)Pb, (234)U and (238)U were determined in umbrella and oral arms of three widely distributed jellyfish species; namely Rhopilema nomadica Galil, 1990, Aurelia aurita Linne, 1758 and Aequorea forskalea Péron & Lesueur, 1810 collected from February 2011 to January 2012 in four sampling locations along the Syrian coast (Eastern Mediterranean Sea). The results have shown significant variations in radionuclides activity concentrations amongst the species. The average activity concentrations of (40)K, (210)Po, (210)Pb, (234)U and (238)U in the umbrella of R. nomadica species were higher than the average activity concentrations in the umbrella of A. aurita species by about 3.2, 1.4, 1.8, 3.2 and 3.2 folds, and A. forskalea species by about 45.5, 15.4, 19, 7.4 and 7.6 folds, respectively. The average activity concentrations of (40)K, (210)Po, (210)Pb, (234)U and (238)U in oral arms of R. nomadica species were higher than the average activity concentrations in oral arms of A. aurita species by about 3.8, 1.7, 1.9, 2.8 and 2.9 folds, respectively. (137)Cs activity concentrations were below the detection limit in all measured samples. In addition, activity concentrations of (137)Cs, (40)K, (210)Po, (210)Pb, (234)U and (238)U were also determined in 44 surface seawater samples and the activity concentrations ranged between 10.6 and 11.9 Bq l(-1) for (40)K, 1.1 and 1.4 mBq l(-1) for (210)Po, 0.5 and 0.7 mBq l(-1) for (210)Pb, 40.8 and 44.5 mBq l(-1) for (234)U, and 36.9 and 38.4 mBq l(-1) for (238)U, while (137)Cs activity concentrations were below the detection limit in all measured samples. Moreover, the umbrella and oral arms readily accumulated (40)K, (210)Po, (210)Pb, (234)U and (238)U above ambient seawater levels in the sequence of (210)Po > (210)Pb > (4) K > (234)U and (238)U. Concentration ratio (CR) values were relatively high for (210)Po and (210)Pb and reached 10(3) and 10(2), respectively for the jellyfish R. nomadica species compared to A. aurita and A. forskalea species. Therefore, R. nomadica can be used as biomonitor for these two radionuclides in the Eastern Mediterranean Sea. However, the obtained data can be considered the first reported baseline values for radioactivity in jellyfish. Copyright © 2015 Elsevier Ltd. All rights reserved.

Potential effects of alpha-recoil on uranium-series dating of calcrete

USGS Publications Warehouse

Neymark, L.A.

2011-01-01

Evaluation of paleosol ages in the vicinity of Yucca Mountain, Nevada, at the time the site of a proposed high-level nuclear waste repository, is important for fault-displacement hazard assessment. Uranium-series isotope data were obtained for surface and subsurface calcrete samples from trenches and boreholes in Midway Valley, Nevada, adjacent to Yucca Mountain. 230Th/U ages of 33 surface samples range from 1.3 to 423 thousand years (ka) and the back-calculated 234U/238U initial activity ratios (AR) are relatively constant with a mean value of 1.54 ± 0.15 (1σ), which is consistent with the closed-system behavior. Subsurface calcrete samples are too old to be dated by the 230Th/U method. U-Pb data for post-pedogenic botryoidal opal from a subsurface calcrete sample show that these subsurface calcrete samples are older than ~ 1.65 million years (Ma), old enough to have attained secular equilibrium had their U-Th systems remained closed. However, subsurface calcrete samples show U-series disequilibrium indicating open-system behavior of 238U daughter isotopes, in contrast with the surface calcrete, where open-system behavior is not evident. Data for 21 subsurface calcrete samples yielded calculable 234U/238U model ages ranging from 130 to 1875 ka (assuming an initial AR of 1.54 ± 0.15, the mean value calculated for the surface calcrete samples). A simple model describing continuous α-recoil loss predicts that the 234U/238U and 230Th/238U ARs reach steady-state values ~ 2 Ma after calcrete formation. Potential effects of open-system behavior on 230Th/U ages and initial 234U/238U ARs for younger surface calcrete were estimated using data for old subsurface calcrete samples with the 234U loss and assuming that the total time of water-rock interaction is the only difference between these soils. The difference between the conventional closed-system and open-system ages may exceed errors of the calculated conventional ages for samples older than ~ 250 ka, but is negligible for younger soils.

Migration behavior of naturally occurring radionuclides at the Nopal I uranium deposit, Chihuahua, Mexico

NASA Astrophysics Data System (ADS)

Prikryl, James D.; Pickett, David A.; Murphy, William M.; Pearcy, English C.

1997-04-01

Oxidation of pyrite at the Nopal I uranium deposit, Peña Blanca district, Chihuahua, Mexico has resulted in the formation of Fe-oxides/hydroxides. Anomalous U concentrations (i.e. several hundred to several thousand ppm) measured in goethite, hematite, and amorphous Fe-oxyhydroxides in a major fracture that crosscuts the deposit and the absence of U minerals in the fracture suggest that U was retained during secondary mineral growth or sorbed on mineral surfaces. Mobilization and transport of U away from the deposit is suggested by decreasing U concentrations in fracture-infilling materials and in goethite and hematite with distance from the deposit. Greater than unity {234U}/{238U} activity ratios measured in fracture-infilling materials indicate relatively recent ( < 1 Ma) U uptake from fluids that carried excess 234U. Systematic decreases in {234U}/{238U} activity ratios of fracture materials with distance from the deposit suggest a multistage mobilization process, such as remobilization of U from 234U-enriched infill minerals or differential or diminished transport of U-bearing solutions containing excess 234U.

Neutron Capture Cross Sections and Gamma Emission Spectra from Neutron Capture on 234,236,238U Measured with DANCE

NASA Astrophysics Data System (ADS)

Ullmann, J. L.; Mosby, S.; Bredeweg, T. A.; Couture, A. J.; Haight, R. C.; Jandel, M.; Kawano, T.; O'Donnell, J. M.; Rundberg, R. S.; Vieira, D. J.; Wilhelmy, J. B.; Wu, C.-Y.; Becker, J. A.; Chyzh, A.; Baramsai, B.; Mitchell, G. E.; Krticka, M.

2014-05-01

A new measurement of the 238U(n, γ) cross section using a thin 48 mg/cm2 target was made using the DANCE detector at LANSCE over the energy range from 10 eV to 500 keV. The results confirm earlier measurements. Measurements of the gamma-ray emission spectra were also made for 238U(n, γ) as well as 234,236U(n, γ). These measurements help to constrain the radiative strength function used in the cross-section calculations.

Determination of U isotope ratios in sediments using ICP-QMS after sample cleanup with anion-exchange and extraction chromatography.

PubMed

Zheng, Jian; Yamada, Masatoshi

2006-01-15

The determination of uranium is important for environmental radioactivity monitoring, which investigates the releases of uranium from nuclear facilities and of naturally occurring radioactive materials by the coal, oil, natural gas, mineral, ore refining and phosphate fertilizer industries, and it is also important for studies on the biogeochemical behavior of uranium in the environment. In this paper, we describe a quadrupole ICP-MS (ICP-QMS)-based analytical procedure for the accurate determination of U isotope ratios ((235)U/(238)U atom ratio and (234)U/(238)U activity ratio) in sediment samples. A two-stage sample cleanup using anion-exchange and TEVA extraction chromatography was employed in order to obtain accurate and precise (234)U/(238)U activity ratios. The factors that affect the accuracy and precision of U isotope ratio analysis, such as detector dead time, abundance sensitivity, dwell time and mass bias were carefully evaluated and corrected. With natural U, a precision lower than 0.5% R.S.D. for (235)U/(238)U atom ratio and lower than 2.0% R.S.D. for (234)U/(238)U activity ratio was obtained with less than 90 ng uranium. The developed analytical method was validated using an ocean sediment reference material and applied to an investigation into the uranium isotopic compositions in a sediment core in a brackish lake in the vicinity of U-related nuclear facilities in Japan.

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

PubMed

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

2012-11-01

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 (236)U/(238)U 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 (234)U/(238)U and (235)U/(238)U ratios. Experimental results obtained for (236)U/(238)U isotope ratios deviated by less than -2.5% from the certified values. Expanded relative total combined standard uncertainties U(c) (k = 2) of 2.6%, 1.4% and 5.8% were calculated for (234)U/(238)U, (235)U/(238)U and (236)U/(238)U, respectively. Copyright © 2012 Elsevier Ltd. All rights reserved.

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

238,234U contents on Lepomis Cyanellus from San Marcos dam located in a uraniferous area

NASA Astrophysics Data System (ADS)

Lares, Magaly Cabral; Luna-Porres, Mayra Y.; Montero-Cabrera, María E.; Renteria-Villalobos, Marusia

2014-07-01

Fish species are suitable biomonitors of radioisotopes in aquatic systems. In the present study, it was made the determination of uranium isotopic contents on fish fillet (Lepomis Cyanellus) from San Marcos dam which is located in uranium mineralized zone. Uranium activity concentrations (AC) in fish samples were obtained on wet weight (ww), using liquid scintillation. 238U and 234U AC in fish fillet ranged from 0.0004 to 0.0167 Bq kg-1, and from 0.0013 to 0.0394 Bq kg-1, respectively. The activity ratio (234U/overflow="scroll">238U) in fish fillet ranged from 2.2 to 8.8. Lepomis cyanellus from San Marcos dam shows bioaccumulation factor (FB) of 0.6 L kg-1. The results suggest that the Lepomis Cyanellus in environments with high U contents tends to have a greater bioaccumulation compared to others.

Seawater 234U/238U recorded by modern and fossil corals

NASA Astrophysics Data System (ADS)

Chutcharavan, Peter M.; Dutton, Andrea; Ellwood, Michael J.

2018-03-01

U-series dating of corals is a crucial tool for generating absolute chronologies of Late Quaternary sea-level change and calibrating the radiocarbon timescale. Unfortunately, coralline aragonite is susceptible to post-depositional alteration of its primary geochemistry. One screening technique used to identify unaltered corals relies on the back-calculation of initial 234U/238U activity (δ234Ui) at the time of coral growth and implicitly assumes that seawater δ234U has remained constant during the Late Quaternary. Here, we test this assumption using the most comprehensive compilation to date of coral U-series measurements. Unlike previous compilations, this study normalizes U-series measurements to the same decay constants and corrects for offsets in interlaboratory calibrations, thus reducing systematic biases between reported δ234U values. Using this approach, we reassess (a) the value of modern seawater δ234U, and (b) the evolution of seawater δ234U over the last deglaciation. Modern coral δ234U values (145.0 ± 1.5‰) agree with previous measurements of seawater and modern corals only once the data have been normalized. Additionally, fossil corals in the surface ocean display δ234Ui values that are ∼5-7‰ lower during the last glacial maximum regardless of site, taxon, or diagenetic setting. We conclude that physical weathering of U-bearing minerals exposed during ice sheet retreat drives the increase in δ234U observed in the oceans, a mechanism that is consistent with the interpretation of the seawater Pb-isotope signal over the same timescale.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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 oasesmore » 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.« less

Consequences of slow growth for 230Th/U dating of Quaternary opals, Yucca Mountain, NV, USA

USGS Publications Warehouse

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

2000-01-01

Thermal ionization mass-spectrometry 234U/238U and 230Th/238U data are reported for uranium-rich opals coating fractures and cavities within the silicic tuffs forming Yucca Mountain, NV, the potential site of a high-level radioactive waste repository. High uranium concentrations (up to 207 ppm) and extremely high 230Th/232Th activity ratios (up to about 106) make microsamples of these opals suitable for precise 230Th/U dating. Conventional 230Th/U ages range from 40 to greater than 600 ka, and initial 234U/238U activity ratios between 1.03 and 8.2. Isotopic evidence indicates that the opals have not experienced uranium mobility; however, wide variations in apparent ages and initial 234U/238U ratios for separate subsamples of the same outermost mineral surfaces, positive correlation between ages and sample weights, and negative correlation between 230Th/U ages and calculated initial 234U/238U are inconsistent with the assumption that all minerals in a given subsample was deposited instantaneously. The data are more consistent with a conceptual model of continuous deposition where secondary mineral growth has occurred at a constant, slow rate up to the present. This model assumes that individual subsamples represent mixtures of older and younger material, and that calculations using the resulting isotope ratios reflect an average age. Ages calculated using the continuous-deposition model for opals imply average mineral growth rates of less than 5 mm/m.y. The model of continuous deposition also predicts discordance between ages obtained using different radiometric methods for the same subsample. Differences in half-lives will result in younger apparent ages for the shorter-lived isotope due to the greater influence of younger materials continuously added to mineral surfaces. Discordant 14C, 230Th/U and U-Pb ages obtained from outermost mineral surfaces at Yucca Mountain support this model. (C) 2000 Elsevier Science B.V. All rights reserved.

Uranium isotopes in rivers, estuaries and adjacent coastal sediments of western India: their weathering, transport and oceanic budget

NASA Astrophysics Data System (ADS)

Borole, D. V.; Krishnaswami, S.; Somayajulu, B. L. K.

1982-02-01

The two major river systems on the west coast of India, Narbada and Tapti, their estuaries and the coastal Arabian sea sediments have been extensively studied for their uranium concentrations and 238U /238U activity ratios. The 238U concentrations in the aqueous phase of these river systems exhibit a strong positive correlation with the sum of the major cations, σ Na + K + Mg + Ca, and with the HCO 3- ion contents. The abundance ratio of dissolved U to the sum of the major cations in these waters is similar to their ratio in typical crustal rocks. These findings lead us to conclude that 238U is brought into the aqueous phase along with major cations and bicarbonate. The strong positive correlation between 238U and total dissolved salts for selected rivers of the world yield an annual dissolved 238U flux of 0.88 × 10 10g/ yr to the oceans, a value very similar to its removal rate from the oceans, 1.05 × 10 10g/ yr, estimated based on its correlation with HCO 3- contents of rivers. In the estuaries, both 238U and its great-grand daughter 234U behave conservatively beyond chlorosities 0.14 g/l. These data confirm our earlier findings in other Indian estuaries. The behavior of uranium isotopes in the chlorosity zone 0.02-0.14 g/l, was studied in the Narbada estuary in some detail. The results, though not conclusive, seem to indicate a minor removal of these isotopes in this region. Reexamination of the results for the Gironde and Zaire estuaries (Martin et al., 1978a and b) also appear to confirm the conservative behavior of U isotopes in unpolluted estuaries. It is borne out from all the available data that estuaries beyond 0.14 g/l chlorosities act neither as a sink nor as a source for uranium isotopes, the behavior in the low chlorosity zones warrants further detailed investigation. A review of the uranium isotope measurements in river waters yield a discharge weighted-average 238U concentration of 0.22 μg/l with a 234U /238U activity ratio of 1.20 ± 0.06 ismissing. The residence time of uranium isotopes in the oceans estimated from the 238U concentration and the 234U /238U A. R. of the rivers yield conflicting results; the material balance of uranium isotopes in the marine environment still remains a paradox. If the disparity between the results is real, then an additional 234U flux of about 0.25 dpm/cm 2·10 3 yr into the oceans (about 20% of its river supply) is necessitated.

Biological availability of (238)U, (234)U and (226)Ra for wild berries and meadow grasses in natural ecosystems of Belarus.

PubMed

Sokolik, G A; Ovsiannikova, S V; Voinikava, K V; Ivanova, T G; Papenia, M V

2014-01-01

This work is devoted to investigation of behavior of (234)U, (238)U and (226)Ra by determining the soil to plant transfer under different natural conditions such as forest or swamped areas and meadow lands with different soil types. The paper summarizes the data on investigation of uranium and radium uptake by wild berries and natural meadow grasses in the typical conditions of Belarus. Parameters characterizing the biological availability of (234)U, (238)U and (226)Ra for bilberry (Vaccinium myrtillus), lingonberry (Vaccinium viti-idaea), blueberry (Vaccinium iliginosum) and cranberry (Vaccinium oxycoccus palustris) as well as for widely occurring mixed meadow vegetation, which belongs to the sedge-grass or grass-sedge associations and forbs, have been established. In the sites under investigation, the deposition levels of (238+239+240)Pu were less than 0.37 kBq m(-2) and (137)Cs deposition ranged between less than 0.37 and 37 kBq m(-2). It was found that activity concentrations of radionuclides in berries varied in the ranges of 0.037-0.11 for (234)U, 0.036-0.10 for (238)U and 0.11-0.43 Bq kg(-1) for (226)Ra, but in the mixed meadow grasses they were 0.32-4.4, 0.24-3.9 and 0.14-6.9 Bq kg(-1) accordingly. The (234)U/(238)U activity ratios were 1.02 ± 0.01 for wild berries, 1.20 ± 0.09 for underground meadow grasses and 1.02 ± 0.02 for proper soils. The concentration ratios (CRs, dry weight basis) of (234)U and (238)U for mixed meadow grasses were 0.036-0.42 and 0.041-0.46 respectively. The correspondent geometric means (GM) were 0.13 and 0.15 with geometric standard deviations (GSD) of 2.4. The CRs of (226)Ra for meadow grasses were 0.031-1.0 with GM 0.20 and GSD 2.6. The CRs of (234)U, (238)U and (226)Ra for wild berries ranged within 0.0018-0.008 (GM is 0.0034, GSD is 1.8), 0.0018-0.008 (GM is 0.0035, GSD is 1.8) and 0.005-0.033 (GM is 0.016, GSD is 2.1) accordingly. The highest CR values of uranium for mixed meadow grasses were found in the sites with high-moor peat and sandy soils. The lowest CRs for grasses were common to loamy and peat-gley soils. The CRs for the same berry species in the sites with sandy soils exceeded the appropriate CR values in the sites with loamy soils by factors of 3-4 for uranium and 4-6 for radium. The data obtained on radionuclide accumulation by plants were used to estimate the average annual effective doses to the population from radionuclide intake through the "soil - wild berries - man" and "soil - meadow vegetation - animal - cow milk-beef - man" trophic chains. The effective doses resulting from (234)U, (238)U and (226)Ra intake with the wild berries for adults were estimated as 0.02-0.09 μSv y(-1) (GM is 0.044, GSD is 1.6). It was established that only in the territory with (137)Cs deposition of ∼1.0-1.5 kBq m(-2) the doses resulting from (234)U, (238)U and (226)Ra intake with wild berries can be comparable with corresponding doses from (137)Cs. In the territories with higher levels of (137)Cs deposition the doses resulting from its intake with the wild berries are usually over the summarized doses of uranium and (226)Ra. The total doses for adults resulting from uranium and (226)Ra intake with cow milk and beef ranged between 0.2 and 7.2 μSv y(-1) (GM is 2.0; GSD is 2.9) and the doses from (226)Ra usually exceeded the appropriate doses of uranium with a factor of 3-37. In the sites with (137)Cs deposition less than 3.7 kBq m(-2), the doses from (234)U, (238)U and (226)Ra intake with cow milk and beef were assessing as 1.1-7.2 μSv y(-1) and they were usually higher than the doses from (137)Cs, which were assessing as 0.4-3.2 μSv y(-1) for its deposition 2 kBq m(-2). In the territory with (137)Cs deposition 10-20 kBq m(-2) and higher, the internal doses resulting from (137)Cs intake with cow milk and beef (10-50 μSv y(-1)) exceeded the proper doses from natural (234)U, (238)U and (226)Ra. Copyright © 2013 Elsevier Ltd. All rights reserved.

Formation of the 50-Year Element 94 from Deuteron Bombardment of U{sup 238}

DOE R&D Accomplishments Database

Kennedy, J. W.; Perlman, M. L.; Segre, E.; Wahl, A. C.

1942-06-01

It has been shown by bombardment with deuterons of a sample of U{sup 238}, greatly depleted in U{sup 235} and U{sup 234}, that the 50-year 94 activity and 2.0 day 93 activity are formed in approximately the same yield as with the natural mixture of uranium isotopes. The activities are thus shown to arise from the U{sup 238} nucleus, and from considerations of the energy of the compound nucleus (U{sup 238} + d).

234U/238U as a ground-water tracer, SW Nevada-SE California

USGS Publications Warehouse

Ludwig, K. R.; Peterman, Z.E.; Simmons, K.R.; Gutentag, E.D.

1993-01-01

The 234U/238U ratio of uranium in oxidizing ground waters is potentially an excellent ground-water tracer because of its high solubility and insensitivity to chemical reactions. Moreover, recent advances in analytical capability have made possible very precise uranium-isotopic analyses on modest (approx.100 ml) amounts of normal ground water. Preliminary results on waters from SW Nevada/Se California indicate two main mixing trends, but in detail indicate significant complexity requiring three or more main components.

Uranium-234 anomalies in authigenic uranium as a new oxygenation proxy in the Southern Ocean

NASA Astrophysics Data System (ADS)

Hayes, C. T.; Severmann, S.; Anderson, A.

2016-12-01

Authigenic uranium (aU) is a sensitive indicator for suboxic conditions in marine pore waters that has been used to reconstruct past oxygenation conditions or organic matter export. aU suffers, however, from possible post-depositional remobilization or "burn-down" when the depth of the oxygenation front in the sediments undergoes rapid changes. In terms of isotope composition, the 234U/238U activity ratio, or δ234U in per mil notation, of authigenic U will reflect the isotope ratio in seawater (147‰) which has been relatively stable (within 15‰) for at least one ocean residence time of U (about 400 kyr). The δ234U ratio in bulk marine sediments should then reflect the mixture of the seawater ratio and the ratio of detrital U (0‰ or somewhat negative). In careful analysis of bulk δ234U over a peak in aU from Southern Ocean core ODP-1094, I found ratios higher than seawater (up to 250‰), not explainable by isotope mixing of known sources. I propose a new diagenetic effect in which a partial reoxidation of an aU emplacement can cause 234U that has been alpha-recoiled from in-situ 238U decay to diffuse into the aU emplacement. This means that with aU records that may be slightly altered by reoxidation, careful tracking of δ234U will allow proper identification of the depth/size of the original aU emplacement. Therefore, δ234U of aU is a more robust redox tracer than elemental proxies alone. In this presentation, I will recount the evidence for this assertion and lay out future research targets.

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.

Practical issues in discriminating between environmental and occupational sources in a uranium urinalysis bioassay program

DOE Office of Scientific and Technical Information (OSTI.GOV)

Long, M.P.; Carbaugh, E.H.; Fairrow, N.L.

1994-11-01

Workers at two Department of Energy facilities, the Pantex Plant in Texas and the Hanford Site in Washington, are potentially exposed to class Y depleted or natural uranium. Since trace amounts of uranium are naturally present in urine excretion, site bioassay programs must be able to discern occupational exposure from naturally occurring uranium exposure. In 1985 Hanford established a 0.2-{mu}g/d environmental screening level for elemental uranium in urine; the protocol was based on log-normal probability analysis of unexposed workers. A second study of background uranium levels commenced in 1990, and experiences in the field indicated that there seemed to bemore » an excessive number of urine samples with uranium above the screening level and that the environmental screening level should be reviewed. Due to unforeseen problems, that second study was terminated before the complete data could be obtained. Natural uranium in rock (by weight, 99.27% {sup 288}U, 0.72% {sup 235}U, and 0.006% {sup 234}U) has approximately equal activity concentrations of {sup 238}U and {sup 234}U. Earlier studies, summarized by the U.S. Environmental Protection Agency in 51 FR 32068, have indicated that {sup 234}U (via {sup 234}Th) has a greater environmental mobility than {sup 238}U and may well have a higher concentration in ground water. By assuming that the {sup 238}U-to {sup 234}U ratio in the urine of nonoccupationally exposed persons should reflect the ratio of environmental levels, significant occupational exposure to depleted uranium would shift that ratio in favor of {sup 238}U, allowing use of the ratio as a co-indicator of occupational exposure in addition to the isotope-specific screening levels. This approach has been adopted by Pantex. The Pacific Northwest Laboratory is studying the feasibility of applying this method to the natural and recycled uranium mixtures encountered at Hanford. The Hanford data included in this report represent work-in-progress.« less

Weathering processes and dating of soil profiles from São Paulo State, Brazil, by U-isotopes disequilibria.

PubMed

Bonotto, Daniel Marcos; Jiménez-Rueda, Jairo Roberto; Fagundes, Isabella Cruz; Filho, Carlos Roberto Alves Fonseca

2017-01-01

This study reports the use of the U-series radionuclides 238 U and 234 U for dating two soil profiles. The soil horizons developed over sandstones from Tatuí and Pirambóia formations at the Paraná sedimentary basin, São Paulo State, Brazil. Chemical data in conjunction with the 234 U/ 238 U activity ratios (AR's) of the soil horizons allowed investigating the U-isotopes mobility in the shallow oxidizing environment. Kaolinization and laterization processes are taking place in the profiles sampled, as they are especially common in regions characterized by a wet and dry tropical climate and a water table that is close to the surface. These processes are implied by inverse significant correlations between silica and iron in both soil profiles. Iron oxides were also very important to retain uranium in the two sites investigated, helping on the understanding of the weathering processes acting there. 238 U and its progeny 234 U permitted evaluating the processes of physical and chemical alteration, allowing the suggestion of a possible timescale corresponding to the Middle Pleistocene for the development of the more superficial soil horizons. Copyright © 2016 Elsevier Ltd. All rights reserved.

Temporal Variations in 234U/238U Activity Ratios in Four Mississippi River Tributaries

NASA Astrophysics Data System (ADS)

Grzymko, T. J.; Marcantonio, F.

2005-05-01

In 2004 we sampled the four tributaries that are the major contributors to the Mississippi River in terms of water discharge, i.e., the Arkansas, Missouri, Upper Mississippi, and Ohio rivers. Each river was sampled four times over the course of the year at variable levels of discharge in an attempt to constrain the causes of the temporal variations of 234U/238U activity ratios in the lower Mississippi River at New Orleans. The tributary uranium data support the idea that lower river uranium isotope and elemental systematics are controlled by a simple mass balance of the source tributary discharges. Furthermore, the uranium isotope ratios of the individual tributaries show coherent patterns of variability. Specifically, the data obtained from the four sampling trips yielded similar patterns of temporal variation in the 234U/238U activity ratios of all of the rivers, although the absolute values of these ratios were distinctly different from one river to the next. The pattern was such that the highest 234U/238U activity ratios were observed during the highest flow associated with the spring freshet while the lowest ratios occurred during the summer. For example, in the Missouri River, the 234U/238U activity ratios varied from 1.51 (February 12) to 1.37 (April 14) to 1.34 (July 16) to 1.37 (November 12), while in the Ohio River the same ratios varied from 1.36 (February 12) to 1.29 (April 14) to 1.21 (July 16) to 1.23 (November 12). The apparent seasonal pattern of these ratios in each tributary has led to several ideas as to the causes of the observed trends. The first, and most obvious, is that in each individual drainage basin there are various source tributaries that contribute to the uranium isotope systematics of the main stem of the tributary of interest. It follows that the variations in the uranium activity ratios may be caused by spatial variations in the source rock chemistry of the drainage basin. Other more complex scenarios can also be envisioned and will be discussed. For example, we explore the possibility that the highest ratios associated with the spring freshet are a consequence of snow melt and the flushing of 234U from fresh surfaces created via physical weathering associated with the winter freeze-thaw cycles.

U isotopes distribution in the Lower Rhone River and its implication on radionuclides disequilibrium within the decay series.

PubMed

Zebracki, Mathilde; Cagnat, Xavier; Gairoard, Stéphanie; Cariou, Nicolas; Eyrolle-Boyer, Frédérique; Boulet, Béatrice; Antonelli, Christelle

2017-11-01

The large rivers are main pathways for the delivery of suspended sediments into coastal environments, affecting the biogeochemical fluxes and the ecosystem functioning. The radionuclides from 238 U and 232 Th-series can be used to understand the dynamic processes affecting both catchment soil erosion and sediment delivery to oceans. Based on annual water discharge the Rhone River represents the largest river of the Mediterranean Sea. The Rhone valley also represents the largest concentration in nuclear power plants in Europe. A radioactive disequilibrium between particulate 226 Ra (p) and 238 U (p) was observed in the suspended sediment discharged by the Lower Rhone River (Eyrolle et al. 2012), and a fraction of particulate 234 Th was shown to derive from dissolved 238 U (d) (Zebracki et al. 2013). This extensive study has investigated the dissolved U isotopes distribution in the Lower Rhone River and its implication on particulate radionuclides disequilibrium within the decay series. The suspended sediment and filtered river waters were collected at low and high water discharges. During the 4-months of the study, two flood events generated by the Rhone southern tributaries were monitored. In river waters, the total U (d) concentration and U isotopes distribution were obtained through Q-ICP-MS measurements. The Lower Rhone River has displayed non-conservative U-behavior, and the variations in U (d) concentration between southern tributaries were related to the differences in bedrock lithology. The artificially occurring 236 U was detected in the Rhone River at low water discharges, and was attributed to the liquid releases from nuclear industries located along the river. The ( 235 U/ 238 U) (d) activity ratio (=AR) in river waters was representative of the 235 U natural abundance on Earth. The ( 226 Ra/ 238 U) (p) AR in suspended sediment has indicated a radioactive disequilibrium (average 1.3 ± 0.1). The excess of 234 Th in suspended sediment =( 234 Th xs(p) ) was apparent solely at low water discharges. The activity of 234 Th xs(p) was calculated through gamma measurements and ranged from unquantifiable to 56 ± 14 Bq kg -1 . The possibility of using 234 Th as a tracer for the suspended sediment dynamics in large Mediterranean river was then discussed. Copyright © 2017 Elsevier Ltd. All rights reserved.

Crustal subsidence rate off Hawaii determined from sup 234 U/ sup 238 U ages of drowned coral reefs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ludwig, K.R.; Szabo, B.J.; Simmons, K.R.

1991-02-01

A series of submerged coral reefs off northwestern Hawaii was formed during (largely glacial) intervals when the rate of local sea-level rise was less than the maximum upward growth rate of the reefs. Mass-spectrometric {sup 234}U/{sup 238}U ages for samples from six such reefs range from 17 to 475 ka and indicate that this part of the Hawaiian Ridge has been subsiding at a roughly uniform rate of 2.6 mm/yr for the past 475 ka. The {sup 234}U/{sup 238}U ages are in general agreement with model ages of reef drowning (based on estimates of paleo-sea-level stands derived from oxygen-isotope ratiosmore » of deep-sea sediments), but there are disagreements in detail. The high attainable precision ({plus minus}10 ka or better on samples younger than {approximately}800 ka), large applicable age range, relative robustness against open-system behavior, and ease of analysis for this technique hold great promise for future applications of dating of 50-1,000 ka coral.« less

Uranium-series dating of pedogenic silica and carbonate, Crater Flat, Nevada

NASA Astrophysics Data System (ADS)

Ludwig, K. R.; Paces, J. B.

2002-02-01

A 230Th-234U-238U dating study on pedogenic silica-carbonate clast rinds and matrix laminae from alluvium in Crater Flat, Nevada was conducted using small-sample thermal-ionization mass spectrometry (TIMS) analyses on a large suite of samples. Though the 232Th content of these soils is not particularly low (mostly 0.1-9 ppm), the high U content of the silica component (mostly 4-26 ppm) makes them particularly suitable for 230Th/U dating on single, 10 to 200 mg totally-digested samples using TIMS. We observed that (1) both micro- (within-rind) and macro-stratigraphic (mappable deposit) order of the 230Th/U ages were preserved in all cases; (2) back-calculated initial 234U/238U fall in a restricted range (typically 1.67±0.19), so that 234U/238U ages with errors of about 100 kyr (2σ) could be reliably determined for the oldest, 400 to 1000 ka rinds; and (3) though 13 of the samples were >350 ka, only three showed evidence for an open-system history, even though the sensitivity of such old samples to isotopic disruption is very high. An attempt to use leach-residue techniques to separate pedogenic from detrital U and Th failed, yielding corrupt 230Th/U ages. We conclude that 230Th/U ages determined from totally dissolved, multiple sub-mm size subsamples provide more reliable estimates of soil chronology than methods employing larger samples, chemical enhancement of 238U/232Th, or isochrons.

Uranium comminution age tested by the eolian deposits on the Chinese Loess Plateau

NASA Astrophysics Data System (ADS)

Li, Le; Liu, Xiangjun; Li, Tao; Li, Laifeng; Zhao, Liang; Ji, Junfeng; Chen, Jun; Li, Gaojun

2017-06-01

The 234U/238U ratio of fine particles can record the time since their separation from bed rock because of the disruption of uranium series equilibrium introduced by the recoil of daughter 234Th nuclei (precursor of 234U) out of particle surfaces during the decay of 238U. Application of the uranium comminution age method, which has great potential in tracing production and transportation of sediments is however complicated by the weathering dissolution of 234U depleted particle surfaces, the difficulty in determining the fraction of recoiled nuclei, and the precipitation of exogenetic 234U. Here we minimize these complications by using a newly developed precise size separation using electroformed sieve, and a chemical protocol that involves reductive and oxidative leaching. Eolian deposits collected from the Chinese Loess Plateau (CLP) were used to test the validity of our method. Possible effects of weathering dissolution were also evaluated by comparing samples with different weathering intensities. The results show decreasing 234U/238U ratios in fine eolian particles with increasing sedimentation age, agreeing well with the theoretical prediction of the comminution age model. This successful application of the uranium comminution age approach to the eolian deposits on the CLP is also aided by a stable dust source, the low weathering intensity, the lack of consolidation, and the well-defined age model of the deposits. A transportation time of 242 ± 18 ka was calculated for the eolian deposits, which indicates a long residence time, and thus extensive mixing, of the dust particles in source regions, partly explaining the stable and homogeneous composition of the eolian dust over glacial-interglacial cycles.

Uranium series dating of Allan Hills ice

NASA Technical Reports Server (NTRS)

Fireman, E. L.

1986-01-01

Uranium-238 decay series nuclides dissolved in Antarctic ice samples were measured in areas of both high and low concentrations of volcanic glass shards. Ice from the Allan Hills site (high shard content) had high Ra-226, Th-230 and U-234 activities but similarly low U-238 activities in comparison with Antarctic ice samples without shards. The Ra-226, Th-230 and U-234 excesses were found to be proportional to the shard content, while the U-238 decay series results were consistent with the assumption that alpha decay products recoiled into the ice from the shards. Through this method of uranium series dating, it was learned that the Allen Hills Cul de Sac ice is approximately 325,000 years old.

U-isotopes and (226)Ra as tracers of hydrogeochemical processes in carbonated karst aquifers from arid areas.

PubMed

Guerrero, José Luis; Vallejos, Ángela; Cerón, Juan Carlos; Sánchez-Martos, Francisco; Pulido-Bosch, Antonio; Bolívar, Juan Pedro

2016-07-01

Sierra de Gádor is a karst macrosystem with a highly complex geometry, located in southeastern Spain. In this arid environment, the main economic activities, agriculture and tourism, are supported by water resources from the Sierra de Gádor aquifer system. The aim of this work was to study the levels and behaviour of some of the most significant natural radionuclides in order to improve the knowledge of the hydrogeochemical processes involved in this groundwater system. For this study, 28 groundwater and 7 surface water samples were collected, and the activity concentrations of the natural U-isotopes ((238)U, (235)U and (234)U) and (226)Ra by alpha spectrometry were determined. The activity concentration of (238)U presented a large variation from around 1.1 to 65 mBq L(-1). Elevated groundwater U concentrations were the result of oxidising conditions that likely promoted U dissolution. The PHREEQC modelling code showed that dissolved U mainly existed as uranyl carbonate complexes. The (234)U/(238)U activity ratios were higher than unity for all samples (1.1-3.8). Additionally, these ratios were in greater disequilibrium in groundwater than surface water samples, the likely result of greater water-rock contact time. (226)Ra presented a wide range of activity concentrations, (0.8 up to about 4 × 10(2) mBq L(-1)); greatest concentrations were detected in the thermal area of Alhama. Most of the samples showed (226)Ra/(234)U activity ratios lower than unity (median = 0.3), likely the result of the greater mobility of U than Ra in the aquifer system. The natural U-isotopes concentrations were strongly correlated with dissolution of sulphate evaporites (mainly gypsum). (226)Ra had a more complex behaviour, showing a strong correlation with water salinity, which was particularly evident in locations where thermal anomalies were detected. The most saline samples showed the lowest (234)U/(238)U activity ratios, probably due to fast uniform bulk mineral dissolution, which would minimize the impact of solubility-controlled fractionation processes. Furthermore, the high bulk dissolution rates promoted greater groundwater (226)Ra/(234)U ratios because the Ra has a comparatively much greater mobility than U in saline conditions. Copyright © 2016 Elsevier Ltd. All rights reserved.

Evaluation of Pleistocene groundwater flow through fractured tuffs using a U-series disequilibrium approach, Pahute Mesa, Nevada, USA

USGS Publications Warehouse

Paces, James B.; Nichols, Paul J.; Neymark, Leonid A.; Rajaram, Harihar

2013-01-01

Groundwater flow through fractured felsic tuffs and lavas at the Nevada National Security Site represents the most likely mechanism for transport of radionuclides away from underground nuclear tests at Pahute Mesa. To help evaluate fracture flow and matrix–water exchange, we have determined U-series isotopic compositions on more than 40 drill core samples from 5 boreholes that represent discrete fracture surfaces, breccia zones, and interiors of unfractured core. The U-series approach relies on the disruption of radioactive secular equilibrium between isotopes in the uranium-series decay chain due to preferential mobilization of 234U relative to 238U, and U relative to Th. Samples from discrete fractures were obtained by milling fracture surfaces containing thin secondary mineral coatings of clays, silica, Fe–Mn oxyhydroxides, and zeolite. Intact core interiors and breccia fragments were sampled in bulk. In addition, profiles of rock matrix extending 15 to 44 mm away from several fractures that show evidence of recent flow were analyzed to investigate the extent of fracture/matrix water exchange. Samples of rock matrix have 234U/238U and 230Th/238U activity ratios (AR) closest to radioactive secular equilibrium indicating only small amounts of groundwater penetrated unfractured matrix. Greater U mobility was observed in welded-tuff matrix with elevated porosity and in zeolitized bedded tuff. Samples of brecciated core were also in secular equilibrium implying a lack of long-range hydraulic connectivity in these cases. Samples of discrete fracture surfaces typically, but not always, were in radioactive disequilibrium. Many fractures had isotopic compositions plotting near the 230Th-234U 1:1 line indicating a steady-state balance between U input and removal along with radioactive decay. Numerical simulations of U-series isotope evolution indicate that 0.5 to 1 million years are required to reach steady-state compositions. Once attained, disequilibrium 234U/238U and 230Th/238U AR values can be maintained indefinitely as long as hydrological and geochemical processes remain stable. Therefore, many Pahute Mesa fractures represent stable hydrologic pathways over million-year timescales. A smaller number of samples have non-steady-state compositions indicating transient conditions in the last several hundred thousand years. In these cases, U mobility is dominated by overall gains rather than losses of U.

U-Th-Ra variations in Himalayan river sediments (Gandak river, India): Weathering fractionation and/or grain-size sorting?

NASA Astrophysics Data System (ADS)

Bosia, Clio; Chabaux, François; Pelt, Eric; France-Lanord, Christian; Morin, Guillaume; Lavé, Jérôme; Stille, Peter

2016-11-01

Understanding the origin of U-Th-Ra variations in the Ganga river sediments is a prerequisite for correctly using U-series nuclides to constrain the sediment transport times in Himalayan rivers. For this purpose, U, Th, and Ra concentrations, along with 238U-234U-230Th-226Ra radioactive disequilibria, were analyzed in bank, bedload and suspended sediments from the Gandak river, one of the main tributaries of the Ganga river. The data confirm that U and Th budgets of the Himalayan sediments are significantly influenced by minor resistant minerals, such as zircon, garnet and Ti-bearing minerals, the dissolution of which required the use of a high-pressure acid digestion process. Most importantly, the results indicate that the variations in (238U/232Th) and (230Th/232Th) activity ratios and 238U-234U-230Th-226Ra disequilibria in sediments along the river alluvial plain mainly reflect modifications in the mineralogical and grain-size compositions rather than the degree of weathering during transport. The (238U/232Th) and (230Th/232Th) activity ratios in the bank and bed sediments are related to variations in the minor primary minerals strongly enriched in U and Th (i.e., zircon, REE-bearing minerals and Ti-bearing minerals), whereas the activity ratios in the suspended load are related to variations in the proportions of clay, Fe-oxyhydroxides and the silt-sand fraction, which contains U- and Th-bearing minor minerals. The data also indicate that 238U-234U-230Th-226Ra disequilibria are strongly influenced by secondary mineral phases: the 230Th budget is likely mainly controlled by Fe-oxyhydroxides, and the 226Ra budget is likely mainly controlled by clay minerals. Therefore, the variations in the 238U-234U-230Th-232Th system in the sediments of the Gandak river cannot simply be interpreted as the result of fractionation due to chemical transformation of the bulk sediment during its transport within the alluvial plain and/or the result of radioactive decay. Consequently, they cannot be used to infer long sediment transport times within the Gandak plain (10-100 ka), as previously proposed. Such analytical and interpretative artifacts are certainly not specific to the present study on the Gandak basin. These issues will certainly be encountered anytime this technique is applied to alluvial systems in which the U and Th budgets of the sediments are influenced by ;heavy; minerals that can be sorted during the transport of sediments within the plain.

238U-234U-230Th disequilibrium in hydrogenous oceanic Fe-Mn crusts: Palaeoceanographic record or diagenetic alteration?

USGS Publications Warehouse

Chabaux, F.; O'Nions, R. K.; Cohen, A.S.; Hein, J.R.

1997-01-01

A detailed TIMS study of (234Uexc/238U), (230Th/232Th), and Th/U ratios have been performed on the outermost margin of ten hydrogenous Fe-Mn crusts from the equatorial Pacific Ocean and west-central Indian Ocean. Th/U concentration ratios generally decrease from the crust's surface down to 0.5-1 mm depth and growth rates estimated by uranium and thorium isotope ratios are significantly different in Fe-Mn crusts from the Peru Basin and the west-central Indian Ocean. Fe-Mn crusts from the same geographical area define a single trend in plots of Ln (234Uexc/238U) vs. Ln(230Th/232Th) and Th/U ratios vs. age of the analysed fractions. Results suggest that (1) hydrogenous Fe-Mn crusts remain closed-systems after formation, and consequently (2) the discrepancy observed between the 230Th and 234U chronometers in Fe-Mn crusts, and the variations of the Th/U ratios through the margin of Fe-Mn crusts, are not due to redistribution of uranium and thorium isotopes after oxyhydroxide precipitation, but rather to temporal variations of both Th/U and initial thorium activity ratios recorded by the Fe-Mn layers. Implications of these observations for determination of Fe-Mn crust growth-rates are discussed. Variations of both Th/U and initial Th activity ratios in Fe-Mn crusts might be related to changes in particle input to seawater and/or changes in ocean circulation during the last 150 ka. Copyright ?? 1997 Elsevier Science Ltd.

Uranium isotopes in well water samples as drinking sources in some settlements around the Semipalatinsk Nuclear Test Site, Kazakhstan.

PubMed

Yamamoto, Masayoshi; Tomita, Junpei; Sakaguchi, Aya; Ohtsuka, Yoshihito; Hoshi, Masaharu; Apsalikov, Kazbek N

Radiochemical results of U isotopes ( 234 U, 235 U and 238 U) and their activity ratios are reported for well waters as local sources of drinking waters collected from the ten settlements around the Semipalatinsk Nuclear Test Site (SNTS), Kazakhstan. The results show that 238 U varies widely from 3.6 to 356 mBq/L (0.3-28.7 μg/L), with a factor of about 100. The 238 U concentrations in some water samples from Dolon, Tailan, Sarzhal and Karaul settlements are comparable to or higher than the World Health Organization's restrictive proposed guideline of 15 μg (U)/L. The 234 U/ 238 U activity ratios in the measured water samples are higher than 1, and vary between 1.1 and 7.9, being mostly from 1.5 to 3. The measured 235 U/ 238 U activity ratios are around 0.046, indicating that U in these well waters is of natural origin. It is probable that the elevated concentration of 238 U found in some settlements around the SNTS is not due to the close-in fallout from nuclear explosions at the SNTS, but rather to the intensive weathering of rocks including U there. The calculated effective doses to adults resulting from consumption of the investigated waters are in the range 1.0-18.7 μSv/y. Those doses are lower than WHO and IAEA reference value (100 μSv/y) for drinking water.

Evaluation of new geological reference materials for uranium-series measurements: Chinese Geological Standard Glasses (CGSG) and macusanite obsidian.

PubMed

Denton, J S; Murrell, M T; Goldstein, S J; Nunn, A J; Amato, R S; Hinrichs, K A

2013-10-15

Recent advances in high-resolution, rapid, in situ microanalytical techniques present numerous opportunities for the analytical community, provided accurately characterized reference materials are available. Here, we present multicollector thermal ionization mass spectrometry (MC-TIMS) and multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS) uranium and thorium concentration and isotopic data obtained by isotope dilution for a suite of newly available Chinese Geological Standard Glasses (CGSG) designed for microanalysis. These glasses exhibit a range of compositions including basalt, syenite, andesite, and a soil. Uranium concentrations for these glasses range from ∼2 to 14 μg g(-1), Th/U weight ratios range from ∼4 to 6, (234)U/(238)U activity ratios range from 0.93 to 1.02, and (230)Th/(238)U activity ratios range from 0.98 to 1.12. Uranium and thorium concentration and isotopic data are also presented for a rhyolitic obsidian from Macusani, SE Peru (macusanite). This glass can also be used as a rhyolitic reference material, has a very low Th/U weight ratio (around 0.077), and is approximately in (238)U-(234)U-(230)Th secular equilibrium. The U-Th concentration data agree with but are significantly more precise than those previously measured. U-Th concentration and isotopic data agree within estimated errors for the two measurement techniques, providing validation of the two methods. The large (238)U-(234)U-(230)Th disequilibria for some of the glasses, along with the wide range in their chemical compositions and Th/U ratios should provide useful reference points for the U-series analytical community.

The estuarine chemistry and isotope systematics of 234,238U in the Amazon and Fly Rivers

USGS Publications Warehouse

Swarzenski, P.; Campbell, P.; Porcelli, D.; McKee, B.

2004-01-01

Natural concentrations of 238U and ??234U values were determined in estuarine surface waters and pore waters of the Amazon and Fly (Papua New Guinea) Rivers to investigate U transport phenomena across river-dominated land-sea margins. Discharge from large, tropical rivers is a major source of dissolved and solid materials transported to the oceans, and are important in defining not only oceanic mass budgets, but also terrestrial weathering rates. On the Amazon shelf, salinity-property plots of dissolved organic carbon, pH and total suspended matter revealed two vastly contrasting water masses that were energetically mixed. In this mixing zone, the distribution of uranium was highly non-conservative and exhibited extensive removal from the water column. Uranium removal was most pronounced within a salinity range of 0-16.6, and likely the result of scavenging and flocculation reactions with inorganic (i.e., Fe/Mn oxides) and organic colloids/particles. Removal of uranium may also be closely coupled to exchange and resuspension processes at the sediment/water interface. An inner-shelf pore water profile indicated the following diagenetic processes: extensive (???1 m) zones of Fe(III) - and, to a lesser degree, Mn(IV) - reduction in the absence of significant S(II) concentrations appeared to facilitate the formation of various authigenic minerals (e.g., siderite, rhodocrosite and uraninite). The pore water dissolved 238U profile co-varied closely with Mn(II). Isotopic variations as evidenced in ??234U pore waters values from this site revealed information on the origin and history of particulate uranium. Only after a depth of about 1 m did the ??234U value approach unity (secular equilibrium), denoting a residual lattice bound uranium complex that is likely an upper-drainage basin weathering product. This suggests that the enriched ??234U values represent a riverine surface complexation product that is actively involved in Mn-Fe diagenetic cycles and surface complexation reactions. In the Fly River estuary, 238U appears to exhibit a reasonably conservative distribution as a function of salinity. The absence of observed U removal does not necessarily imply non-reactivity, but instead may record an integration of concurrent U removal and release processes. There is not a linear correlation between ??234U vs. 1/ 238U that would imply simple two component mixing. It is likely that resuspension of bottom sediments, prolonged residence times in the lower reaches of the Fly River, and energetic particle-colloid interactions contribute to the observed estuarine U distribution. The supply of uranium discharged from humid, tropical river systems to the sea appears to be foremost influenced by particle/water interactions that are ultimately governed by the particular physiographic and hydrologic characteristics of an estuary. ?? 2004 Elsevier Ltd. All rights reserved.

A study on possible use of Urtica dioica (common nettle) plants as uranium (234U, 238U) contamination bioindicator near phosphogypsum stockpile.

PubMed

Olszewski, Grzegorz; Boryło, Alicja; Skwarzec, Bogdan

The aim of this study was to determine uranium concentrations in common nettle ( Urtica dioica ) plants and corresponding soils samples which were collected from the area of phosphogypsum stockpile in Wiślinka (northern Poland). The uranium concentrations in roots depended on its concentrations in soils. Calculated BCF and TF values showed that soils characteristics and air deposition affect uranium absorption and that different uranium species have different affinities to U . dioica plants. The values of 234 U/ 238 U activity ratio indicate natural origin of these radioisotopes in analyzed plants. Uranium concentration in plants roots is negatively weakly correlated with distance from phosphogypsum stockpile.

Natural radionuclide mobility and its influence on U-Th-Pb dating of secondary minerals from the unsaturated zone at Yucca Mountain, Nevada

USGS Publications Warehouse

Neymark, L.A.; Amelin, Y.V.

2008-01-01

Extreme U and Pb isotope variations produced by disequilibrium in decay chains of 238U and 232Th are found in calcite, opal/chalcedony, and Mn-oxides occurring as secondary mineral coatings in the unsaturated zone at Yucca Mountain, Nevada. These very slowly growing minerals (mm my-1) contain excess 206Pb and 208Pb formed from excesses of intermediate daughter isotopes and cannot be used as reliable 206Pb/238U geochronometers. The presence of excess intermediate daughter isotopes does not appreciably affect 207Pb/235U ages of U-enriched opal/chalcedony, which are interpreted as mineral formation ages. Opal and calcite from outer (younger) portions of coatings have 230Th/U ages from 94.6 ?? 3.7 to 361.3 ?? 9.8 ka and initial 234U/238U activity ratios (AR) from 4.351 ?? 0.070 to 7.02 ?? 0.12, which indicate 234U enrichment from percolating water. Present-day 234U/238U AR is ???1 in opal/chalcedony from older portions of the coatings. The 207Pb/235U ages of opal/chalcedony samples range from 0.1329 ?? 0.0080 to 9.10 ?? 0.21 Ma, increase with microstratigraphic depth, and define slow long-term average growth rates of about 1.2-2.0 mm my-1, in good agreement with previous results. Measured 234U/238U AR in Mn-oxides, which pre-date the oldest calcite and opal/chalcedony, range from 0.939 ?? 0.006 to 2.091 ?? 0.006 and are >1 in most samples. The range of 87Sr/86Sr ratios (0.71156-0.71280) in Mn-oxides overlaps that in the late calcite. These data indicate that Mn-oxides exchange U and Sr with percolating water and cannot be used as a reliable dating tool. In the U-poor calcite samples, measured 206Pb/207Pb ratios have a wide range, do not correlate with Ba concentration as would be expected if excess Ra was present, and reach a value of about 1400, the highest ever reported for natural Pb. Calcite intergrown with opal contains excesses of both 206Pb and 207Pb derived from Rn diffusion and from direct ??-recoil from U-rich opal. Calcite from coatings devoid of opal/chalcedony contains 206Pb and 208Pb excesses, but no appreciable 207Pb excesses. Observed Pb isotope anomalies in calcite are explained by Rn-produced excess Pb. The Rn emanation may strongly affect 206Pb-238U ages of slow-growing U-poor calcite, but should be negligible for dating fast-growing U-enriched speleothem calcite.

Drastic shifts in the Levant hydroclimate during the last interglacial indicate changes in the tropical climate and winter storm tracks

NASA Astrophysics Data System (ADS)

Kiro, Y.; Goldstein, S. L.; Kushnir, Y.; Lazar, B.; Stein, M.

2017-12-01

Marine Isotope Stage (MIS) 5e was a warm interglacial with where with significantly varying insolation and hence varied significantly throughout this time suggesting highly variable climate. The ICDP Dead Sea Deep Drilling Project recovered a 460m record of the past 220ka, reflecting the variable climate along MIS 5e. This time interval is reflected by alternating halite and detritus sequences, including 20m of halite-free detritus during the peak insolation at 125 ka. The Dead Sea salt budget indicates that the Levant climate was extremely arid when halite formed, reaching 20% of the present runoff. The halite-free detritus layer reflects increased precipitation to levels similar to present day, assuming similar spatial and temporal rainfall patterns. However, the 234U/238U activity ratio in the lake, reflected by authigenic minerals (aragonite, gypsum and halite), shifts from values of 1.5 (reflecting the Jordan River, the present main water source) down to 1.3 at 125-122ka during the MIS5e insolation peak and 1.0 at 118-116ka. The low 234U/238U reflects increased flash floods and eastern water sources (234U/238U 1.05-1.2) from the drier part of the watershed in the desert belt. The intermediate 234U/238U of 1.3 suggests that the Jordan River, fed from Mediterranean-sourced storm tracks, continued to flow along with an increase in southern and eastern water sources. NCAR CCSM3 climate model runs for 125ka indicate increases in both Summer and Winter precipitation. The drastic decrease to 234U/238U 1.0 occurs during the driest period, indicating a near shutdown of Jordan River flow, and water input only through flash floods and southern and eastern sources. The 120ka climate model runs shows a decrease in Winter and increase in Fall precipitation as a result of an increased precipitation in the tropics. The extreme aridity, associated with increased flooding is similar to patterns expected due to future warming. The increase in aridity is the result of expansion of the desert-belt and increases in southern precipitation and indicates an important link between the tropical and mid-latitude climate.

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.

Uranium and plutonium in anoxic marine sediments of the Santiago River mouth (Eastern Pacific, Mexico).

PubMed

Almazán-Torres, María Guadalupe; Ordóñez-Regil, Eduardo; Ruiz-Fernández, Ana Carolina

2016-11-01

The uranium (U) and plutonium (Pu) content with depth in a sediment core collected in the continental shelf off the mouth of the Santiago River in the Mexican Pacific was studied to evaluate the contamination effects of the effluent of the Santiago-Lerma River as it moves into the sea. The large mass of terrestrial detritus delivered by the river influences the physicochemical and geochemical processes in the seafloor. Abnormal concentrations of U and Pu in sediments were examined as indicative of the effects of anoxic conditions. One of the indicators of pollution of seawater is the bacterial activity of the shallow seabed layer; and among the prevailing bacteria, the magnetotactic ones induce the formation of euhedral and framboidal shapes (pyrite). These pyrite entities are by-products of anoxic environments loaded with decomposing detrital material and are very abundant in the surface layers of the sediment core analyzed. The pyrite formation is the result of a biochemical reaction between iron and organic sulphur reduced by bacteria, and the pyrite entities precipitate to the seafloor. In the same upper zone of the profile, 238 U is readily immobilized, while 234 U is oxidized and dissolved in seawater by the effect of hot atom chemistry. This may cause the activity ratio (AR) 234 U/ 238 U disequilibrium (near 0.41). Furthermore, in the shallow layer of the sediment core, an abnormally high concentration of 239+240 Pu was detected. In this upper layer, the activity concentrations found were 3.19 Bq kg -1 for 238 U, 1.32 kg -1 for 234 U and 2.78 Bq kg -1 for 239+240 Pu. In the lower fractions of the sediment core, normal values of AR 234 U/ 238 U (≈1) were found, with traces of 239+240 Pu. Copyright © 2016 Elsevier Ltd. All rights reserved.

Connecting the U-Th and U-Pb Chronometers: New Algorithms and Applications

NASA Astrophysics Data System (ADS)

McLean, N. M.; Smith, C. J. M.; Roberts, N. M. W.; Richards, D. A.

2016-12-01

The U-Th and U-Pb geochronometers are important clocks for separate intervals of the geologic timescale. U-Th dates exploit disequilibrium in the 238U intermediate daughter isotopes 234U and 230Th, and are often used to date corals and speleothems that are zero age through 800 ka. The U-Pb system relies on secular equilibrium decay of 238U to 206Pb and 235U to 207Pb over longer timescales, and can be used to date samples from <1 Ma to 4.5 Ga. Disequilibrium plays a role in young U-Pb dates, but only as a nuisance correction. Both chronometers can produce dates with uncertainties <0.1% near the center of their applicable age ranges, but become less precise at their intersection, when the 238U decay chain approaches secular equilibrium and there has been little time for ingrowth of radiogenic Pb. However, if measurements or assumptions about both chronometers can be made, then they can be combined into a single, more informed date. Coupling the datasets can improve their precision and accuracy and help interrogate the assumptions that underpin each. Working with this data is difficult for two reasons. The Bateman equations are long and cumbersome for U decay chains that include 238U, 234U, 230Th, 226Ra, 206Pb and 235U, 231Pa, and 207Pb. Also, Pb measurements often comprise varying amounts of radiogenic Pb from locally heterogeneous U concentrations mixed with varying amounts of common Pb. At present there is no established, flexible computational framework to combine information from measurements and/or assumptions of these parameters, and no way to visualize and interpret the results. We present new algorithms to quickly and accurately solve the system of differential equations defined by both of the uranium decay chains and the linear regression through the U-Pb isochron. The results are illustrated on a new concordia diagram, where the concordia curve is determined by measured and/or assumed U-series disequilibrium and can have unfamiliar topologies. We demonstrate this approach using data collected by solution and laser ablation ICPMS on carbonates with measurable 230Th and 234U disequilibrium, measurable disequilibrium for only 234U, and when only assumptions can be made about initial U-series disequilibrium. Potential applications include refining chronologies at ca. 1 Ma, an important period in Earth history.

Non-destructive determination of uranium, thorium and 40K in tobacco and their implication on radiation dose levels to the human body.

PubMed

Landsberger, S; Lara, R; Landsberger, S G

2015-11-01

The naturally occurring radionuclides of (235)U, (238)U and (232)Th and their daughter products are a potential major source of anthropogenic radiation to tobacco smokers. Often overlooked is the presence of (40)K in tobacco and its implication to radiation dose accumulation in the human body. In this study, these three radiation sources have been determined in four typical US cigarettes using neutron activation analysis (NAA). The NAA reactions of (238)U(n,γ)(239)U, (232)Th(n,γ)(233)Th and (41)K(n,γ)(42)K were used to determine (235)U, (238)U and (232)Th and (40)K, respectively. The activity of (238)U can easily be determined by epithermal NAA of the (238)U(n,γ)(239)U reaction, and the activity of (235, 234)U can easily be deduced. Using isotopic ratios, the activity due to (40)K was found by the determined concentrations of (41)K (also by epithermal neutrons) in the bulk material. Each gram of total potassium yields 30 Bq of (40)K. The annual effective dose for smokers using 20 cigarettes per day was calculate to be 14.6, 137 and 9 μSv y(-1) for (238,235,) (234)U, (232)Th and (40)K, respectively. These values are significantly lower that the dose received from (210)Po except for (232)Th. © The Author 2015. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

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

DOE PAGES

Brown, Shaun T.; Basu, Anirban; Christensen, John N.; ...

2016-05-20

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 bymore » approximately 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

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, Robert G.

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 fluctuations in climate, fire disturbance and vegetation. Radiocarbon (14C) analysis of dissolved organic carbon (DOC) in thaw waters supports ages greater than ∼40 ky BP below 10 m. DOC concentrations in thaw waters increased with depth to maxima of >1000 ppm, despite little change in ice content or cryostructures. These relations suggest time-dependent production of old DOC that will be released upon permafrost thaw at a rate that is mediated by sediment transport, among other factors.

Radionuclide concentrations in benthic invertebrates from Amchitka and Kiska Islands in the Aleutian Chain, Alaska.

PubMed

Burger, Joanna; Gochfeld, Michael; Jewett, Stephen C

2007-05-01

Concentrations of 13 radionuclides (137Cs, 129I, 60Co, 152Eu, 90Sr, 99Tc, 241Am, 238Pu, 239,249Pu, 234U, 235U, 236U, 238U) were examined in seven species of invertebrates from Amchitka and Kiska Islands, in the Aleutian Chain of Alaska, using gamma spectroscopy, inductively coupled plasma mass spectroscopy, and alpha spectroscopy. Amchitka Island was the site of three underground nuclear test (1965-1971), and we tested the null hypotheses that there were no differences in radionuclide concentrations between Amchitka and the reference site (Kiska) and there were no differences among species. The only radionuclides where composite samples were above the Minimum Detectable Activity (MDA) were 137Cs, 241Am, 239,249Pu, 234U, 235U, 236U, and 238U. Green sea urchin (Strongylocentrotus polyacanthus), giant chiton (Cryptochiton stelleri), plate limpets (Tectura scutum) and giant Pacific octopus (Enteroctopus dofleini) were only tested for 137Cs; octopus was the only species with detectable levels of 137Cs (0.262 +/- 0.029 Bq/kg, wet weight). Only rock jingle (Pododesmus macroschisma), blue mussel (Mytilus trossulus) and horse mussel (Modiolus modiolus) were analyzed for the actinides. There were no interspecific differences in 241Am and 239,240Pu, and almost no samples above the MDA for 238Pu and 236U. Horse mussels had significantly higher concentrations of 234U (0.844 +/- 0.804 Bq/kg) and 238U (0.730 +/- 0.646) than the other species (both isotopes are naturally occurring). There were no differences in actinide concentrations between Amchitka and Kiska. In general, radionuclides in invertebrates from Amchitka were similar to those from uncontaminated sites in the Northern Hemisphere, and below those from the contaminated Irish Sea. There is a clear research need for authors to report the concentrations of radionuclides by species, rather than simply as 'shellfish', for comparative purposes in determining geographical patterns, understanding possible effects, and for estimating risk to humans from consuming different biota.

Spatially-Resolved Analyses of Aerodynamic Fallout from a Uranium-Fueled Nuclear Test

DOE PAGES

Lewis, L. A.; Knight, K. B.; Matzel, J. E.; ...

2015-07-28

The fiive silicate fallout glass spherules produced in a uranium-fueled, near-surface nuclear test were characterized by secondary ion mass spectrometry, electron probe microanalysis, autoradiography, scanning electron microscopy, and energy-dispersive x-ray spectroscopy. Several samples display compositional heterogeneity suggestive of incomplete mixing between major elements and natural U ( 238U/ 235U = 0.00725) and enriched U. Samples exhibit extreme spatial heterogeneity in U isotopic composition with 0.02 < 235U/ 238U < 11.84 among all five spherules and 0.02 < 235U/ 238U < 7.41 within a single spherule. Moreover, in two spherules, the 235U/ 238U ratio is correlated with changes in major elementmore » composition, suggesting the agglomeration of chemically and isotopically distinct molten precursors. Two samples are nearly homogenous with respect to major element and uranium isotopic composition, suggesting extensive mixing possibly due to experiencing higher temperatures or residing longer in the fireball. Linear correlations between 234U/ 238U, 235U/ 238U, and 236U/ 238U ratios are consistent with a two-component mixing model, which is used to illustrate the extent of mixing between natural and enriched U end members.« less

Investigation of the /sup 234/U//sup 238/U disequilibrium in the natural waters of the Santa Fe River basin north-central Florida

DOE Office of Scientific and Technical Information (OSTI.GOV)

Briel, L.I.

1976-01-01

Typical surface water masses in the Santa Fe basin are characterized by a /sup 238/U concentration of 0.224 +- .014 ppB and a /sup 234/U//sup 238/U activity ratio of 1.081 +- .038. The Floridan aquifer in this area is represented by at least two distinct regimes of ground water. The effluent from the Poe Springs group has a nominal uranium concentration of 0.938 +- .014 ppB and an activity ratio of 0.900 +- .012, while the effluent from the Ichetucknee Springs group has a nominal uranium concentration of 0.558 +- .018 ppB and an activity ratio of 0.707 +- .022.more » The effluent from ten additional springs in the Santa Fe system can be represented by hypothetical mixtures of these two ground water regimes and a hypothetical surface water component, which may reflect the extent of local recharge to the aquifer in different parts of the basin.« less

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.

Environmental characterization and radio-ecological impacts of non-nuclear industries on the Red Sea coast.

PubMed

El Mamoney, M H; Khater, Ashraf E M

2004-01-01

The Red Sea is a deep semi-enclosed and narrow basin connected to the Indian Ocean by a narrow sill in the south and to the Suez Canal in the north. Oil industries in the Gulf of Suez, phosphate ore mining activities in Safaga-Quseir region and intensified navigation activities are non-nuclear pollution sources that could have serious radiological impacts on the marine environment and the coastal ecosystems of the Red Sea. It is essential to establish the radiological base-line data, which does not exist yet, and to investigate the present radio-ecological impact of the non-nuclear industries to preserve and protect the coastal environment of the Red Sea. Some natural and man-made radionuclides have been measured in shore sediment samples collected from the Egyptian coast of the Red Sea. The specific activities of 226Ra and 210Pb (238U) series, 232Th series, 40K and 137Cs (Bq/kg dry weight) were measured using gamma ray spectrometers based on hyper-pure germanium detectors. The specific activities of 210Po (210Pb) and uranium isotopes (238U, 235U and 234U) (Bq/kg dry weight) were measured using alpha spectrometers based on surface barrier (PIPS) detectors after radiochemical separation. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of 228Ra/226Ra, 210Pb/226Ra, 226Ra/238U and 234U/238U were calculated for evaluation of the geo-chemical behaviour of these radionuclides. The average specific activity of 226Ra (238U) series, 232Th series, 40K and 210Pb were 24.7, 31.4, 427.5 and 25.6 Bq/kg, respectively. The concentration of 137Cs in the sediment samples was less than the lower limit of detection. The Red Sea coast is an arid region with very low rainfall and the sediment is mainly composed of sand. The specific activity of 238U, 235U and 234U were 25.3, 2.9 and 25.0 Bq/kg. The average specific activity ratios of 226Ra/228Ra, 210Pb/226Ra and 234U/238U were 1.67, 1.22 and 1.0, respectively. The relationship between 226Ra/228Ra activity ratio and sample locations along the coastal shoreline indicates the increase of this ratio in the direction of the Shuqeir in the north and Safaga in the south where the oil exploration and phosphate mining activities are located. These activities may contribute a high flux of 226Ra. The concentration and distribution pattern of 226Ra in sediment can be used to trace the radiological impact of the non-nuclear industries on the Red Sea coast.

Ground water contamination with (238)U, (234)U, (235)U, (226)Ra and (210)Pb from past uranium mining: cove wash, Arizona.

PubMed

Dias da Cunha, Kenya Moore; Henderson, Helenes; Thomson, Bruce M; Hecht, Adam A

2014-06-01

The objectives of the study are to present a critical review of the (238)U, (234)U, (235)U, (226)Ra and (210)Pb levels in water samples from the EPA studies (U.S. EPA in Abandoned uranium mines and the Navajo Nation: Red Valley chapter screening assessment report. Region 9 Superfund Program, San Francisco, 2004, Abandoned uranium mines and the Navajo Nation: Northern aum region screening assessment report. Region 9 Superfund Program, San Francisco, 2006, Health and environmental impacts of uranium contamination, 5-year plan. Region 9 Superfund Program, San Franciso, 2008) and the dose assessment for the population due to ingestion of water containing (238)U and (234)U. The water quality data were taken from Sect. "Data analysis" of the published report, titled Abandoned Uranium Mines Project Arizona, New Mexico, Utah-Navajo Lands 1994-2000, Project Atlas. Total uranium concentration was above the maximum concentration level for drinking water (7.410-1 Bq/L) in 19 % of the water samples, while (238)U and (234)U concentrations were above in 14 and 17 % of the water samples, respectively. (226)Ra and (210)Pb concentrations in water samples were in the range of 3.7 × 10(-1) to 5.55 × 102 Bq/L and 1.11 to 4.33 × 102 Bq/L, respectively. For only two samples, the (226)Ra concentrations exceeded the MCL for total Ra for drinking water (0.185 Bq/L). However, the (210)Pb/(226)Ra ratios varied from 0.11 to 47.00, and ratios above 1.00 were observed in 71 % of the samples. Secular equilibrium of the natural uranium series was not observed in the data record for most of the water samples. Moreover, the (235)U/(total)U mass ratios ranged from 0.06 to 5.9 %, and the natural mass ratio of (235)U to (total)U (0.72 %) was observed in only 16 % of the water samples, ratios above or below the natural ratio could not be explained based on data reported by U.S. EPA. In addition, statistical evaluations showed no correlations among the distribution of the radionuclide concentrations in the majority of the water samples, indicating more than one source of contamination could contribute to the sampled sources. The effective doses due to ingestion of the minimum uranium concentrations in water samples exceed the average dose considering inhalation and ingestion of regular diet for other populations around the world (1 μSv/year). The maximum doses due to ingestion of (238)U or (234)U were above the international limit for effective dose for members of the public (1 mSv/year), except for inhabitants of two chapters. The highest effective dose was estimated for inhabitants of Cove, and it was almost 20 times the international limit for members of the public. These results indicate that ingestion of water from some of the sampled sources poses health risks.

Environmental control of U concentration and 234U/238U in speleothems at subannual resolution

NASA Astrophysics Data System (ADS)

Hu, C.; Henderson, G. M.

2003-12-01

Trace element and isotope variability in speleothems encodes a range of information about the past environment, although its interpretation is often problematic. U concentration and isotopes have frequently been analysed in speleothems in order to provide chronology, but their use as environmental proxies in their own right has not been comprehensively investigated. In this study, we have investigated the environmental controls of U in a stalagmite from the Central Yangtze Valley in China. This stalagmite grew rapidly throughout the Holocone and contains visible annual layers about 300microns thick. Analysis of a portion of the stalagmite corresponding to the 1970s by electron probe, LA-ICP-MS, and by physical subsampling indicate clear annual cycles in Sr/Ca, Mg/Ca, and Ba/Ca. The reasonably open cave structure and the correlation of Sr/Ca with Mg/Ca suggest that temperature exerts considerable control over these trace element variations. U/Ca also varies seasonally by up to 42 % and shows a clear anti-correlation with Mg/Ca (correlation coefficient -0.64). Based on the inverse relationship between U/Ca and temperature exhibited in other carbonates (e.g. corals) the speleothem U/Ca is suggested to be controlled primarily by temperature and may provide a paleo cave thermometer with less rainfall influence than Mg/Ca. Ongoing monitoring of the cave temperature and humidity will assess the robustness of this conclusion and the sensitivity of speleothem U/Ca to temperature. (234U/238U) in this stalagmite range from 1.733 to 1.872 during the Holocene. The U concentration is high enough (typically 0.48 ppm) and growth rate fast enough, that (234U/238U) can also be measured at a subannual resolution. The expected alpha-recoil control of excess 234U supply suggests that these measurements may provide a measure of the transit time of recharge waters to the stalagmite during the seasonal cycle. Such a proxy would enable deconvolution of temperature and recharge-rate control in trace element records from speleothems.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ku, T. L.; Luo, S.; Goldstein, S. J.

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 leadsmore » 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.« less

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.

Extended optical model for fission

DOE PAGES

Sin, M.; Capote, R.; Herman, M. W.; ...

2016-03-07

A comprehensive formalism to calculate fission cross sections based on the extension of the optical model for fission is presented. It can be used for description of nuclear reactions on actinides featuring multi-humped fission barriers with partial absorption in the wells and direct transmission through discrete and continuum fission channels. The formalism describes the gross fluctuations observed in the fission probability due to vibrational resonances, and can be easily implemented in existing statistical reaction model codes. The extended optical model for fission is applied for neutron induced fission cross-section calculations on 234,235,238U and 239Pu targets. A triple-humped fission barrier ismore » used for 234,235U(n,f), while a double-humped fission barrier is used for 238U(n,f) and 239Pu(n,f) reactions as predicted by theoretical barrier calculations. The impact of partial damping of class-II/III states, and of direct transmission through discrete and continuum fission channels, is shown to be critical for a proper description of the measured fission cross sections for 234,235,238U(n,f) reactions. The 239Pu(n,f) reaction can be calculated in the complete damping approximation. Calculated cross sections for 235,238U(n,f) and 239Pu(n,f) reactions agree within 3% with the corresponding cross sections derived within the Neutron Standards least-squares fit of available experimental data. Lastly, the extended optical model for fission can be used for both theoretical fission studies and nuclear data evaluation.« less

Concentration and characteristics of depleted uranium in water, air and biological samples collected in Serbia and Montenegro.

PubMed

Jia, Guogang; Belli, Maria; Sansone, Umberto; Rosamilia, Silvia; Gaudino, Stefania

2005-09-01

During the Balkan conflicts, in 1995 and 1999, depleted uranium (DU) rounds were employed and were left in the battlefield. Health concern is related to the risk arising from contamination of the environment with DU penetrators and dust. In order to evaluate the impact of DU on the environment and population in Serbia and Montenegro, radiological surveys of DU in water, air and biological samples were carried out over the period 27 October-5 November 2001. The uranium isotopic concentrations in biological samples collected in Serbia and Montenegro, mainly lichens and barks, were found to be in the range of 0.67-704 Bqkg(-1) for (238)U, 0.48-93.9 Bqkg(-1) for (234)U and 0.02-12.2 Bqkg(-1) for (235)U, showing uranium levels to be higher than in the samples collected at the control sites. Moreover, (236)U was detectable in some of the samples. The isotopic ratios of (234)U/(238)U showed DU to be detectable in many biological samples at all examined sites, especially in Montenegro, indicating widespread ground-surface DU contamination, albeit at very low level. The uranium isotopic concentrations in air obtained from the air filter samples collected in Serbia and Montenegro were found to be in the range of 1.99-42.1 microBqm(-3) for (238)U, 0.96-38.0 microBqm(-3) for (234)U, and 0.05-1.83 microBqm(-3) for (235)U, being in the typical range of natural uranium values. Thus said, most of the air samples are DU positive, this fact agreeing well with the widespread DU contamination detected in the biological samples. The uranium concentrations in water samples collected in Serbia and Montenegro were found to be in the range of 0.40-21.9 mBql(-1) for (238)U, 0.27-28.1 mBql(-1) for (234)U, and 0.01-0.88 mBql(-1) for (235)U, these values being much lower than those in mineral water found in central Italy and below the WHO guideline for drinking water. From a radiotoxicological point of view, at this moment there is no significant radiological risk related to these investigated sites in terms of possible DU contamination of water, air and/or plants.

The fission cross sections of /sup 230/Th, /sup 232/Th, /sup 233/U, /sup 234/U, /sup 236/U, /sup 238/U, /sup 237/Np, /sup 239/Pu and /sup 242/Pu relative /sup 235/U at 14. 74 MeV neutron energy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meadows, J.W.

1986-12-01

The measurement of the fission cross section ratios of nine isotopes relative to /sup 235/U at an average neutron energy of 14.74 MeV is described with particular attention to the determination of corrections and to sources of error. The results are compared to ENDF/B-V and to other measurements of the past decade. The ratio of the neutron induced fission cross section for these isotopes to the fission cross section for /sup 235/U are: /sup 230/Th - 0.290 +- 1.9%; /sup 232/Th - 0.191 +- 1.9%; /sup 233/U - 1.132 +- 0.7%; /sup 234/U - 0.998 +- 1.0%; /sup 236/U -more » 0.791 +- 1.1%; /sup 238/U - 0.587 +- 1.1%; /sup 237/Np - 1.060 +- 1.4%; /sup 239/Pu - 1.152 +- 1.1%; /sup 242/Pu - 0.967 +- 1.0%. 40 refs., 11 tabs., 9 figs.« less

Chemical and U-Sr isotopic variations of stream and source waters at a small catchment scale (the Strengbach case; Vosges mountains; France)

NASA Astrophysics Data System (ADS)

Pierret, M. C.; Stille, P.; Prunier, J.; Viville, D.; Chabaux, F.

2014-03-01

This is the first comprehensive study dealing with major and trace element data as well as 87Sr/86Sr isotope and (234U/238U) activity ratios (AR) determined on the totality of springs and brooks of the Strengbach catchment. It shows that the small and more or less monolithic catchment drains different sources and streamlets with very different isotopic and geochemical signatures. Different parameters control the diversity of the source characteristics. Of importance is especially the hydrothermal overprint of the granitic bedrock, which was stronger for the granite from the northern than from the southern slope; also significant are the different meteoric alteration processes of the bedrock causing the formation of 0.5 to 9 m thick saprolite and above the formation of an up to 1 m thick soil system. These processes mainly account for springs and brooks from the northern slope having higher Ca/Na, Mg/Na, Sr/Na ratios but lower 87Sr/86Sr isotopic ratios than those from the southern slope. The chemical compositions of the source waters in the Strengbach catchment are only to a small extent the result of alteration of primary bedrock minerals and rather reflect dissolution/precipitation processes of secondary mineral phases like clay minerals. The (234U/238U) AR, however, are decoupled from the 87Sr/86Sr isotope system and reflect to some extent the level of altitude of the source and, thus, the degree of alteration of the bedrock. The sources emerging at high altitudes have circulated through already weathered materials (saprolite and fractured rock depleted in 234U) implying (234U/238U) AR < 1, which is uncommon for surface waters. Preferential flow paths along constant fractures in the bedrocks might explain the over time homogeneous U AR of the different spring waters. However, the geochemical and isotopic variations of stream waters at the outlet of the catchment are controlled by variable contributions of different springs depending on the hydrological conditions. It appears that the (234U/238U) AR is an appropriate very important tracer for studying and deciphering the contribution of the different source fluxes at the catchment scale because this unique geochemical parameter is different for each individual spring and at the same time remains unchanged for each of the springs with changing discharge and fluctuating hydrological conditions. This study further highlights the important impact of different and independent water pathways in fractured granite controlling the different geochemical and isotopic signatures of the waters.

Method for radioactivity monitoring

DOEpatents

Umbarger, C. John; Cowder, Leo R.

1976-10-26

The disclosure relates to a method for analyzing uranium and/or thorium contents of liquid effluents preferably utilizing a sample containing counting chamber. Basically, 185.7-keV gamma rays following .sup.235 U alpha decay to .sup.231 Th which indicate .sup.235 U content and a 63-keV gamma ray doublet found in the nucleus of .sup.234 Pa, a granddaughter of .sup.238 U, are monitored and the ratio thereof taken to derive uranium content and isotopic enrichment .sup.235 U/.sup.235 U + .sup.238 U) in the liquid effluent. Thorium content is determined by monitoring the intensity of 238-keV gamma rays from the nucleus of .sup.212 Bi in the decay chain of .sup.232 Th.

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.

Measuring Uranium Decay Rates for Advancement of Nuclear Forensics and Geochronology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parsons-Davis, Tashi

Radioisotopic dating techniques are highly valuable tools for understanding the history of physical and chemical processes in materials related to planetary sciences and nuclear forensics, and rely on accurate knowledge of decay constants and their uncertainties. The decay constants of U-238 and U-235 are particularly important to Earth science, and often the measured values with lowest reported uncertainties are applied, although they have not been independently verified with similar precision. New direct measurements of the decay constants of U-238, Th-234, U-235, and U-234 were completed, using a range of analytical approaches. An overarching goal of the project was to ensuremore » the quality of results, including metrological traceability to facilitate implementation across diverse disciplines. This report presents preliminary results of these experiments, as a few final measurements and calculations are still in progress.« less

Age of the moon: An isotopic study of uranium-thorium-lead systematics of lunar samples

USGS Publications Warehouse

Tatsumoto, M.; Rosholt, J.N.

1970-01-01

Concentrations of U, Th, and Pb in Apollo 11 samples studied are low (U. 0.16 to 0.87; Th, 0.53 to 3.4; Pb, 0.29 to 1.7, in ppm) but the extremely radiogenic lead in samples allows radiometric dating. The fine dust and the breccia have a concordant age of 4.66 billion years on the basis of 207Pb/206Pb, 206Pb/238U, 207Pb/235U, and 208Pb/232Th ratios. This age is comparable with the age of meteorites and with the age generally accepted for the earth. Six crystalline and vesicular samples are distinctly younger than the dust and breccia. The 238U/235U ratio is the same as that in earth rocks, and 234U is in radioactive equilibrium with parent 238U.

Determination of natural radioactivity in irrigation water of drilled wells in northwestern Saudi Arabia.

PubMed

Alkhomashi, N; Al-Hamarneh, Ibrahim F; Almasoud, Fahad I

2016-02-01

The levels of natural radiation in bedrock groundwater extracted from drilled wells in selected farms in the northwestern part of Saudi Arabia were addressed. The investigated waters form a source of irrigation for vegetables, agricultural crops, wheat, and alfalfa to feed livestock consumed by the general public. Information about water radioactivity in this area is not available yet. Therefore, this study strives to contribute to the quality assessment of the groundwater of these wells that are drilled into the non-renewable Saq sandstone aquifer. Hence, gross alpha and beta activities as well as the concentrations of (224)Ra, (226)Ra, (228)Ra, (234)U, (238)U, and U(total) were measured, compared to national and international limits and contrasted with data quoted from the literature. Correlations between the activities of the analyzed radionuclides were discussed. The concentrations of gross alpha and beta activities as well as (228)Ra were identified by liquid scintillation counting whereas alpha spectrometry was used to determine (224)Ra, (226)Ra, (234)U and (238)U after separation from the matrix by extraction chromatography. The mean activity concentrations of gross α and β were 3.15 ± 0.26 Bq L(-1) and 5.39 ± 0.44 Bq L(-1), respectively. Radium isotopes ((228)Ra and (226)Ra) showed mean concentrations of 3.16 ± 0.17 Bq L(-1) and 1.12 ± 0.07 Bq L(-1), respectively, whereas lower levels of uranium isotopes ((234)U and (238)U) were obtained. Copyright © 2015 Elsevier Ltd. All rights reserved.

Transformation of Upland Water and Carbon Dynamics by Thawing Permafrost in the Alaskan Interior

NASA Astrophysics Data System (ADS)

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

2009-05-01

Large arctic rivers can provide an integrated signal of regional permafrost thaw and associated carbon dynamics. A long-term (30-y) decrease in dissolved organic carbon (DOC) and increase in dissolved inorganic carbon in the Yukon River Basin (YRB) suggest increased flow through mineral soils as a result of permafrost thaw. We used U series isotopes to test for the influence of thaw on soil and surface waters in small upland catchments at two sites within the YRB. In natural waters, 234U/238U activity ratios exceed 1.00 (secular equilibrium) as a function of water-rock contact time. Previous work has shown that in major YRB rivers, seasonally and spatially variable 234U/238U ratios could indicate both groundwater inputs and permafrost thaw, with ratios ranging from 1.1 to 2.6. We show that 234U/238U ratios in soil and surface water from these small catchments span the range of values observed in the major rivers, and indicate greater influence of older water where the mineral soil and underlying sediment facilitate drainage and permafrost degradation. Analysis of deep, ice-rich loess permafrost cores (2-10 m) reveals that thaw of Pleistocene ice can release high concentrations of DOC (>1000 ppm) and ammonium in thaw waters. The age and chemical composition of these waters allows for improved prediction of downstream carbon dynamics upon thaw. Field observation of hillslope soil sequences indicates that both topography and mineral substrate influence the effects of thaw on water and carbon dynamics in small catchments.

Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers

DOE PAGES

Kayzar, Theresa M.; Williams, Ross W.

2015-09-26

The model age or ‘date of purification’ of a nuclear material is an important nuclear forensic signature. In this study, chemical separation and MC-ICP-MS measurement techniques were developed for 226 Ra and 227Ac: grand-daughter nuclides in the 238U and 235U decay chains respectively. The 230Th- 234U, 226Ra- 238U, 231Pa- 235U, and 227Ac- 235U radiochronometers were used to calculate model ages for CRM-U100 standard reference material and two highly-enriched pieces of uranium metal from the International Technical Working Group Round Robin 3 Exercise. In conclusion, the results demonstrate the accuracy of the 226Ra- 238U and 227Ac- 235U chronometers and provide informationmore » about nuclide migration during uranium processing.« less

Developing 226Ra and 227Ac age-dating techniques for nuclear forensics to gain insight from concordant and non-concordant radiochronometers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kayzar, Theresa M.; Williams, Ross W.

The model age or ‘date of purification’ of a nuclear material is an important nuclear forensic signature. In this study, chemical separation and MC-ICP-MS measurement techniques were developed for 226 Ra and 227Ac: grand-daughter nuclides in the 238U and 235U decay chains respectively. The 230Th- 234U, 226Ra- 238U, 231Pa- 235U, and 227Ac- 235U radiochronometers were used to calculate model ages for CRM-U100 standard reference material and two highly-enriched pieces of uranium metal from the International Technical Working Group Round Robin 3 Exercise. In conclusion, the results demonstrate the accuracy of the 226Ra- 238U and 227Ac- 235U chronometers and provide informationmore » about nuclide migration during uranium processing.« less

Assessment of the vertical distribution of natural radionuclides in a mineralized uranium area in south-west Spain.

PubMed

Blanco Rodríguez, P; Vera Tomé, F; Lozano, J C

2014-01-01

Low-level alpha spectrometry techniques using semiconductor detectors (PIPS) and liquid scintillation (LKB Quantulus 1220™) were used to determine the activity concentration of (238)U, (234)U, (230)Th, (226)Ra, (232)Th, and (210)Pb in soil samples. The soils were collected from an old disused uranium mine located in southwest Spain. The soils were sampled from areas with different levels of influence from the installation and hence had different levels of contamination. The vertical profiles of the soils (down to 40 cm depth) were studied in order to evaluate the vertical distribution of the natural radionuclides. To determine the origin of these natural radionuclides the Enrichment Factor was used. Also, study of the activity ratios between radionuclides belonging to the same radioactive series allowed us to assess the different types of behaviors of the radionuclides involved. The vertical profiles for the radionuclide members of the (238)U series were different at each sampling point, depending on the level of influence of the installation. However, the profiles of each point were similar for the long-lived radionuclides of the (238)U series ((238)U, (234)U, (230)Th, and (226)Ra). Moreover, a major imbalance was observed between (210)Pb and (226)Ra in the surface layer, due to (222)Rn exhalation and the subsequent surface deposition of (210)Pb. Copyright © 2013 Elsevier Ltd. All rights reserved.

Radiogenic isotopic approaches for quantifying radionuclide transport (Invited)

NASA Astrophysics Data System (ADS)

Maher, K.; Depaolo, D. J.; Singleton, M. J.; Christensen, J. N.; Conrad, M. E.

2009-12-01

Naturally occurring variations in the isotopic compositions of U and Sr provide unique opportunities for assessing the fate and transport of radionuclides at field-scale conditions. When coupled with reactive transport models, U and Sr isotopes may also provide additional constraints on the rates of sediment-fluid or sediment-waste interactions. Such isotopic approaches can be useful for sites where subsurface characterization is complicated by a lack of accessibility or the presence of substantial heterogeneity. In addition, a variety of quantitative modeling approaches of different complexity can be used to evaluate experimentally determined parameters for radionuclide mobility at the field-scale. At the Hanford Site in eastern Washington, 87Sr/86Sr and 234U/238U ratios have been used to quantify the residence time of Sr and U in the unsaturated zone, the long-term background infiltration rate through the unsaturated zone, and to assess the influence of enhanced wastewater discharge on the regional unconfined aquifer. As a result of different processing techniques or due to interactions between caustic waste and the natural sediment, waste plumes may also inherit isotopic fingerprints (e.g. 234U/238U, 235U/238U, 236U/238U; δ15N & δ18O of nitrate) that can be used to resolve multiple sources of contamination. Finally, enriched isotopic tracers can be applied to experimental manipulations to assess the retardation of a variety of contaminants. Collectively this isotopic data contributes unique perspectives on both the hydrologic conditions across the site and the mobility of key radionuclides. Predicting the long-term fate and transport of radionuclides in the environment is often challenging due to natural heterogeneity and incomplete characterization of the subsurface, however detailed analysis of isotopic variations can provide one additional means of characterizing the subsurface.

Saprolite Formation Rates using U-series Isotopes in a Granodiorite Weathering Profile from Boulder Creek CZO (Colorado, USA)

NASA Astrophysics Data System (ADS)

Pelt, Eric; Chabaux, Francois; Mills, T. Joseph; Anderson, Suzanne P.; Foster, Melissa A.

2015-04-01

Timescales of weathering profile formation and evolution are important kinetic parameters linked to erosion, climatic, and biological processes within the critical zone. In order to understand the complex kinetics of landscape evolution, water and soil resources, along with climate change, these parameters have to be estimated for many different contexts. The Betasso catchment, within the Boulder Creek Critical Zone Observatory (BC-CZO) in Colorado, is a mountain catchment in Proterozoic granodiorite uplifted in the Laramide Orogeny ca. 50 Ma. In an exposure near the catchment divide, an approximately 1.5 m deep profile through soil and saprolite was sampled and analysed for bulk U-series disequilibria (238U-234U-230Th-226Ra) to estimate the profile weathering rate. The (234U/238U), (230Th/234U) and (226Ra/230Th) disequilibria through the entire profile are small but vary systematically with depth. In the deepest samples, values are close to equilibrium. Above this, values are progressively further from equilibrium with height in the profile, suggesting a continuous leaching of U and Ra compared to Th. The (234U/238U) disequilibria remain < 1 along the profile, suggesting no significant U addition from pore waters. Only the shallowest sample (~20 cm depth) highlights a 226Ra excess, likely resulting from vegetation cycling. In contrast, variations of Th content and (230Th/232Th) - (238U/232Th) activity ratios in the isochron diagram are huge, dividing the profile into distinct zones above and below 80 cm depth. Below 80 cm, the Th content gradually increases upward from 1.5 to 3.5 ppm suggesting a relative accumulation linked to chemical weathering. Above 80 cm, the Th content jumps to ~15 ppm with a similar increase of Th/Ti or Th/Zr ratios that clearly excludes the same process of relative accumulation. This strong shift is also observed in LREE concentrations, such as La, Ce and Nd, and in Sr isotopic composition, which suggests an external input of radiogenic material such as dust from the western Colorado deserts or eroding landscapes. For the deeper part of the profile, the strong upward decrease of the (230Th/232Th) and (238U/232Th) activity ratio without generation of strong disequilibria could suggest a long history (~0.5-1 Ma) of U leaching with a very slow saprolite development (~1 m/Ma). Such a result is in agreement with slow weathering rates deduced from modern solute chemistry of rivers, but would be much lower than 10Be denudation rates on the same profile of ~10-20 m/Ma. As the 10Be rates integrate denudation over a timescale of 40-80 ka, the apparent inconsistency between rates deduced by U-series data and Be data might suggest that erosion rates have increased during the 10Be integrating time.

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.

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.

Uranium isotopes in tree bark as a spatial tracer of environmental contamination near former uranium processing facilities in southwest Ohio.

PubMed

Conte, Elise; Widom, Elisabeth; Kuentz, David

2017-11-01

Inappropriate handling of radioactive waste at nuclear facilities can introduce non-natural uranium (U) into the environment via the air or groundwater, leading to anthropogenic increases in U concentrations. Uranium isotopic analyses of natural materials (e.g. soil, plants or water) provide a means to distinguish between natural and anthropogenic U in areas near sources of radionuclides to the environment. This study examines the utility of two different tree bark transects for resolving the areal extent of U atmospheric contamination using several locations in southwest Ohio that historically processed U. This study is the first to utilize tree bark sampling transects to assess environmental contamination emanating from a nuclear facility. The former Fernald Feed Materials Production Center (FFMPC; Ross, Ohio) produced U metal from natural U ores and recycled nuclear materials from 1951 to 1989. Alba Craft Laboratory (Oxford, Ohio) machined several hundred tons of natural U metal from the FFMPC between 1952 and 1957. The Herring-Hall-Marvin Safe Company (HHM; Hamilton, Ohio) intermittently fabricated slugs rolled from natural U metal stock for use in nuclear reactors from 1943 to 1951. We have measured U concentrations and isotope signatures in tree bark sampled along an ∼35 km SSE-NNW transect from the former FFMPC to the vicinity of the former Alba Craft laboratories (transect #1) and an ∼20 km SW- NE (prevailing local wind direction) transect from the FFMPC to the vicinity of the former HHM (transect #2), with a focus on old trees with thick, persistent bark that could potentially record a time-integrated signature of environmental releases of U related to anthropogenic activity. Our results demonstrate the presence of anthropogenic U contamination in tree bark from the entire study area in both transects, with U concentrations within 1 km of the FFMPC up to ∼400 times local background levels of 0.066 ppm. Tree bark samples from the Alba Craft and HHM transects exhibit increasing U concentrations within ∼5 and ∼10 km, respectively of the FFMPC. The 236 U/ 238 U isotopic ratios in tree bark from both transects increase progressively towards the FFMPC with values as high as 2.00 × 10 -4  at the FFMPC. Tree bark sampled within 1 km of the FFMPC exhibits clear evidence for both enriched and depleted uranium with 235 U/ 238 U values from 0.00461 to 0.00736, with 234 U/ 238 U activity ratio ranging from 0.53 to 0.96, and 236 U/ 238 U from 6.05 × 10 -5 to 1.05 × 10 -4 . Tree bark from transect #1 between 1 and 30 km from the FFMPC exhibits depleted and natural 235 U/ 238 U values ranging from 0.00552 to 0.00726 [ 234 U/ 238 U activity ratio: 0.69-1.04; 236 U/ 238 U: 2.49 × 10 -6 - 2.00 × 10 -4 ]. Tree bark from transect #2 sampled between 1 and ∼20 km away from the FFMPC exhibits evidence of enriched and depleted U in the environment with 235 U/ 238 U ranging from 0.00635 to 0.00738 [ 234 U/ 238 U activity ratio: 0.83-0.98; 236 U/ 238 U: 1.43 × 10 -5 - 2.00 × 10 -4 ]. Results from scanning electron microscopy with energy dispersive spectrometry provides evidence for U-rich particles as the source of contamination found in tree bark growing within 1-3 km of the former FFMPC. Such observations are consistent with the previously observed 14 μm U-rich particle identified in tree bark sampled within 1 km of the FFMPC (Conte et al., 2015). Overall, this study shows the usefulness of a tree bark sample transect to assess the areal extent of atmospheric contaminant U stemming from nuclear facilities. Copyright © 2017 Elsevier Ltd. All rights reserved.

Development of a Scalable Process Control System for Chemical Soil Washing to Remove Uranyl Oxide

DTIC Science & Technology

2015-05-01

ICET also has a fully equipped counting laboratory for the evaluation of radioactive samples . Photographs of the 1-meter and 3-meter motorized...the leachate will be monitored using a gamma detector. There are numerous naturally occurring radioactive materials in soil . ICET has developed a...48.6% from 238U and 49.2% from 234U. The 238U in NU also contains daughters that are radioactive . This increases the activity of samples over long

Constraining the calculation of U 234 , 236 , 238 ( n , γ ) cross sections with measurements of the γ -ray spectra at the DANCE facility

DOE PAGES

Ullmann, J. L.; Kawano, T.; Baramsai, B.; ...

2017-08-31

The cross section for neutron capture in the continuum region has been difficult to calculate accurately. Previous results for 238 U show that including an M 1 scissors-mode contribution to the photon strength function resulted in very good agreement between calculation and measurement. Our paper extends that analysis to 234 , 236 U by using γ -ray spectra measured with the Detector for Advanced Neutron Capture Experiments (DANCE) at the Los Alamos Neutron Science Center to constrain the photon strength function used to calculate the capture cross section. Calculations using a strong scissors-mode contribution reproduced the measured γ -ray spectramore » and were in excellent agreement with the reported cross sections for all three isotopes.« less

Applications of New Synthetic Uranium Reference Materials for Research in Geochemistry

NASA Astrophysics Data System (ADS)

Richter, Stephan; Alonso, Adolfo; Aregbe, Yetunde; Eykens, Roger; Jacobsson, Ulf; Kuehn, Heinz; Verbruggen, Andre; Weyer, Stefan

2010-05-01

For many applications in geochemistry research isotope ratio measurements play a significant role. In geochronology isotope abundances of uranium and its daughter products thorium and lead are being used to determine the age and history of various samples of geological interest. For measuring the isotopic compositions of these elements by mass spectrometry, suitable isotope reference materials are needed to validate measurement procedures and to calibrate multi-collector and ion counting detector systems. IRMM is a recognized provider for nuclear isotope reference materials to the nuclear industry and nuclear safeguards authorities, which are also being applied widely for geochemical applications. Firstly, the double spike IRMM-3636 with a 233U/236U ratio of 1:1 was prepared which allows internal mass fractionation correction for high precision 235U/238U ratio measurements. The 234U abundance of this double spike material is low enough to allow an accurate and precise correction of 234U/238U ratios, even for measurements of close to equilibrium uranium samples. The double spike IRMM-3636 is offered in 3 concentrations: 1mg/g, 0.1mg/g and 0.005mg/g. Secondly, the 236U single spike IRMM-3660 was prepared and is offered in 3 concentrations: 1mg/g, 0.1mg/g and 0.01mg/g. Thirdly, a "Quad"-isotope reference material, IRMM-3101, has been prepared which is characterized by 233U/235U/236U/238U=1/1/1/1. This material is useful for checking Faraday cup efficiencies and inter-calibration of MIC (multiple ion counting) detectors. The quad-IRM is offered in 3 concentrations: 1mg/g, 0.1mg/g and 0.01mg/g. As one example for the significant influence of synthetic reference materials for geochemical research, the IRMM-074 series of gravimetrically prepared uranium mixtures for linearity testing of secondary electron multipliers (SEMs) has been applied for the redetermination of the secular equilibrium 234U/238U value and the 234U half-life by Cheng et al (2009). Due to the use of IRMM-074, results with smaller uncertainties were obtained, which are shifted by about 0.04% compared to the commonly used values published earlier by Cheng et al. in 2000. This has a significant impact for U isotope measurements in geochemistry. As another example for a geochemical application, by using the new double spike IRMM-3636, the 235U/238U ratios for several commonly used natural U standard materials from NIST/NBL and IRMM, such as e.g. NBS960 (=NBL CRM-112a), NBS950a,b and IRMM-184, have been re-measured at IRMM and other laboratories with improved precision and accuracy. The (preliminary) new result of 137.839(24) for the 238U/235U ratio of NBL CRM-112a is deviating by -0.030% from the well-known and widely used old consensus value of 137.88. For this old consensus value no uncertainty has ever been assigned, but it is outside the uncertainty limits of the new measurement result. The new result is based on measurements made at several laboratories worldwide, such as University of Frankfurt (Germany), National Taiwan University, NERC (University of Nottingham, UK), UNM (University of Minnesota, US), Thermo Fisher Scientific, LLNL (Lawrence Livermore National Laboratory, US.DOE), SAL/IAEA and IRMM. The (preliminary) new result of 137.839(24) can therefore be proposed as a new consensus value for the 238U/235U ratio of NBL CRM-112a. In contrast to the older consensus value, this new result is traceable to the common SI system of units and has an uncertainty assigned to it. For the close to natural standard IRMM-184, the re-measured 238U/235U ratio of 137.683(23) agrees quite well with the certified value of 137.697(41), the calculated difference is only -0.010(35)% which is insignificant. As a conclusion, the IRMM-3636 Double Spike has been successfully applied for measurements of important uranium isotopic standards like NBL CRM-112a and IRMM-184, with improved uncertainties at the level of 0.016% and traceability to the SI system.

Environmental assessment of gamma-radiation levels in stream sediments around Sharm El-Sheikh, South Sinai, Egypt.

PubMed

Al-Sharkawy, A; Hiekal, M Th; Sherif, M I; Badran, H M

2012-10-01

A total surface area of ∼170 km(2) including 28 localities around Sharm El-Sheikh, South Sinai, were investigated by γ-ray spectroscopy. The concentrations of NORM were found to be five to seven-fold that in dune sands in different regions in Sinai. While relatively higher levels of (238)U, (234)Th, (226)Ra, and (232)Th are associated with the existing monzo-syenogranite, the concentration of (40)K is more uniformly distributed in the studied area. Locations with higher concentrations of (137)Cs are mainly located in the northern part. The (238)U, (234)Th and (226)Ra isotopes in the (238)U-series are in secular equilibrium. The absorbed dose rates and gamma-radiation hazard indices in all locations were higher than the world average value and unity, respectively. Properly regulated land use is recommended for a buffer zone in the northern part of the study area. Copyright © 2012 Elsevier Ltd. All rights reserved.

Quantifying weathering advance rates in basaltic andesite rinds with uranium-series isotopes: a case study from Guadeloupe

NASA Astrophysics Data System (ADS)

Ma, L.; Chabaux, F. J.; Pelt, E.; Granet, M.; Sak, P. B.; Gaillardet, J.; Brantley, S. L.

2010-12-01

Weathering of basaltic rocks plays an important role in many Earth surface processes. It is thus of great interest to quantify their weathering rates. Because of their well-documented behaviors during water-rock interaction, U-series isotopes have been shown to have utility as a potential chronometer to constrain the formation rates of weathering rinds developed on fresh basaltic rocks. In this study, U-series isotopes and trace element concentrations were analyzed in a basaltic andesite weathering rind collected from the Bras David watershed, Guadeloupe. From the clast, core and rind samples were obtained by drilling along a 63.8 mm linear profile across a low curvature segment of the core-rind boundary. Trace element concentrations reveal: significant loss of REE, Y, Rb, Sr, and Ba in the weathering rind; conservative behaviors of Ti and Th; and external addition of U into the rind during clast weathering. Measured (234U/238U) activity ratios of the rind samples are much higher than the core samples and show excess 234U. Measured (238U/232Th) and (230Th/232Th) activity ratios of the core and rind samples increase gradually from the core into the weathering rind. The observed depletion profiles for the trace elements in the clast suggest that the earliest chemical reaction that creates significant porosity is dissolution of plagioclase, consistent with the previous study [Sak et al., 2010, CG, in press]. The porosity growth within the rind allows for an influx of soil solution that carries dissolved U with (234U/238U) activity ratios >1 into the clast. The deposition of U in the rind is most likely associated with precipication of secondary minerals during clast weathering. Such a continuous U addition is responsible for the observed gradual increase of (238U/232Th) activity ratios in the rind. Subsequent production of 230Th in the rind over time from the decay of excess 234U accounts for the observed continuous increase of (230Th/232Th) activity ratios. The U-series activity ratios in the clast were modeled with a weathering advance rate of ~0.3 mm kyr-1. This represents the rind advance rate at the low curvature segment of the core-rind boundary under tropical climate. This rate is consistent with the previously estimated formation rates of basaltic rinds under similar tropic conditions in Costa Rica [Sak et al., 2004, GCA 68, 1453; Pelt et al., 2008, EPSL 276, 98]. This rate is about one order of magnitude greater than those in temperate regions, documenting the important control of temperature on basalt weathering. This work illustrates that the weathering advance rates of rinds can be successfully estimated by U-series isotopes, demonstrating their great potential as dating tools for Earth surface processes. Furthermore, U-series chronometry provides a suitable method for independently testing the hypothesis that rind advance rates around an individual clast increase with increasing interfacial curvature.

Isotopic Clues on Factors Controlling Geochemical Fluxes From Large Watersheds in Eastern Canada

NASA Astrophysics Data System (ADS)

Rosa, E.; Helie, J.; Ghaleb, B.; Hillaire-Marcel, C.; Gaillardet, J.

2008-12-01

A monitoring and monthly sampling program of the Nelson, Ottawa, St. Lawrence, La Grande and Great Whale rivers was started in September 2007. It provides information on the seasonality and sources of geochemical fluxes into the Hudson Bay and the North Atlantic from watersheds covering more than 2.6 106 km2 of the eastern Canadian boreal domain. Measurements of pH and alkalinity, analyses of major ions, strontium and dissolved silica, 2H and 18O of water, concentrations and isotopic properties of dissolved organic and inorganic carbon (13C) and uranium (234U/238U) were performed. Lithology more than latitudinal climatic gradients controls the river geochemistry. Rivers draining silicate terrains show lower dissolved U concentrations but greater 234U/238U disequilibria than rivers draining carbonates (average of 1.38 vs. 1.23). Groundwater supplies might exert some control on these U- isotope signatures. No clear seasonality is observed in 234U/238U ratios, but U concentrations are correlated to dissolved organic carbon (DOC) concentrations in most rivers. Rivers draining carbonates present higher total dissolved carbon concentrations and higher 13C-contents in dissolved inorganic carbon (DIC), in response to the dissolution of soil carbonates. DOC/DIC ratios above 2.4 are observed in rivers draining silicates; their lower 13C-DIC content directly reflects the organic matter oxidation in soils. Total dissolved solids are one order of magnitude or more greater in rivers draining carbonates, showing the strong difference in chemical weathering rates according to the geological setting. The stability in chemical fluxes and water isotopic compositions in the La Grande River, which hosts hydroelectric reservoirs covering more than 12 000 km2, indicates that it is the most buffered hydrological system among the investigated watersheds. Seasonal fluctuations are observed elsewhere, with maximum geochemical fluxes during the spring snowmelt. 2H-18O content of river water appears to be the only parameter presenting a strong latitudinal and climatic gradient (independent of lithology).

Chemical and U-Sr isotopic variations in stream and source waters of the Strengbach watershed (Vosges mountains, France)

NASA Astrophysics Data System (ADS)

Pierret, M. C.; Stille, P.; Prunier, J.; Viville, D.; Chabaux, F.

2014-10-01

This is the first comprehensive study dealing with major and trace element data as well as 87Sr/86Sr isotope and (234U/238U) activity ratios (AR) determined on the totality of springs and brooks of the Strengbach catchment. It shows that the small and more or less monolithic catchment drains different sources and streamlets with very different isotopic and geochemical signatures. Different parameters control the diversity of the source characteristics. Of importance is especially the hydrothermal overprint of the granitic bedrock, which was stronger for the granite from the northern slope; also significant are the different meteoric alteration processes of the bedrock causing the formation of 0.5 to 9 m thick saprolite and above the formation of an up to 1m thick soil system. These processes mainly account for springs and brooks from the northern slope having higher Ca / Na, Mg / Na, and Sr / Na ratios, but lower 87Sr/86Sr isotopic ratios than those from the southern slope. The chemical compositions of the source waters in the Strengbach catchment are only to a small extent the result of alteration of primary bedrock minerals, and rather reflect dissolution/precipitation processes of secondary mineral phases like clay minerals. The (234U/238U) AR, however, are decoupled from the 87Sr/86Sr isotope system, and reflect to some extent the level of altitude of the source and, thus, the degree of alteration of the bedrock. The sources emerging at high altitudes have circulated through already weathered materials (saprolite and fractured bedrock depleted in 234U), implying (234U/238U) AR below 1, which is uncommon for surface waters. Preferential flow paths along constant fractures in the bedrocks might explain the - over time - homogeneous U AR of the different spring waters. However, the geochemical and isotopic variations of stream waters at the outlet of the catchment are controlled by variable contributions of different springs, depending on the hydrological conditions. It appears that the (234U/238U) AR are a very appropriate, important tracer for studying and deciphering the contribution of the different source fluxes at the catchment scale, because this unique geochemical parameter is different for each individual spring and at the same time remains unchanged for each of the springs with changing discharge and fluctuating hydrological conditions. This study further highlights the important impact of different and independent water pathways on fractured granite controlling the different geochemical and isotopic signatures of the waters. Despite the fact that soils and vegetation cover have a great influence on the water cycle balance (evapotranspiration, drainage, runoff), the chemical compositions of waters are strongly modified by processes occurring in deep saprolite and bedrock rather than in soils along the specific water pathways.

Regolith production rates calculated with uranium-series isotopes at Susquehanna/Shale Hills Critical Zone Observatory

NASA Astrophysics Data System (ADS)

Ma, Lin; Chabaux, Francois; Pelt, Eric; Blaes, Estelle; Jin, Lixin; Brantley, Susan

2010-08-01

In the Critical Zone where rocks and life interact, bedrock equilibrates to Earth surface conditions, transforming to regolith. The factors that control the rates and mechanisms of formation of regolith, defined here as material that can be augered, are still not fully understood. To quantify regolith formation rates on shale lithology, we measured uranium-series (U-series) isotopes ( 238U, 234U, and 230Th) in three weathering profiles along a planar 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 and element transport, i.e., the relative mobility decreases in the order 234U > 238U > 230Th. The activity ratios observed in the regolith samples are explained by i) loss of U-series isotopes during water-rock interactions and ii) re-deposition of U-series isotopes downslope. Loss of U and Th initiates in the meter-thick zone of "bedrock" that cannot be augered but that nonetheless consists of up to 40% clay/silt/sand inferred to have lost K, Mg, Al, and Fe. Apparent equivalent regolith production rates calculated with these isotopes for these profiles decrease exponentially from 45 m/Myr to 17 m/Myr, with increasing regolith thickness from the ridge top to the valley floor. With increasing distance from the ridge top toward the valley, apparent equivalent regolith residence times increase from 7 kyr to 40 kyr. Given that the SSHO experienced peri-glacial climate ˜ 15 kyr ago and has a catchment-wide averaged erosion rate of ˜ 15 m/Myr as inferred from cosmogenic 10Be, we conclude that the hillslope retains regolith formed before the peri-glacial period and is not at geomorphologic steady state. Both chemical weathering reactions of clay minerals and translocation of fine particles/colloids are shown to contribute to mass loss of U and Th from the regolith, consistent with major element data at SSHO. This research documents a case study where U-series isotopes are used to constrain the time scales of chemical weathering and regolith production rates. Regolith production rates at the SSHO should be useful as a reference value for future work at other weathering localities.

U, Th, and Pb isotopes in hot springs on the Juan de Fuca Ridge

NASA Technical Reports Server (NTRS)

Chen, J. H.

1987-01-01

Concentrations and isotopic compositions of U, Th, and Pb in three hydrothermal fluids from the Juan de Fuca Ridge were determined from samples obtained by the Alvin submersible. The samples were enriched in Pb and Th relative to deep-sea water, and were deficient in U. No clear relationship with Mg was found, suggesting nonideal mixing between the hot hydrothermal fluids and the cold ambient seawater. Values for U-234/U-238 have a seawater signature, and show a U-234 enrichment relative to the equilibrium value. The Pb isotopic composition has a uniform midocean ridge basalt signature, and it is suggested that Pb in these fluids may represent the best average value of the local oceanic crust.

Evaluation of processes occurring in the bottom nepheloid layer (BNL) of an eastern Mediterranean area using 234Th/238U disequilibria.

PubMed

Evangeliou, Nikolaos; Florou, Heleny

2013-09-01

Particle-reactive radionuclide (234)Th and its ratios with the conservative (238)U were used to trace the marine processes occurring over short timescales in the bottom nepheloid layer (BNL) of seven stations in the Saronikos Gulf and the Elefsis Bay (Greece) during three seasons (summer 2008, autumn 2008 and winter 2009). Summer was considered as a steady season where low physical processes occur and stratification is well established, autumn as a commutative period and winter as period of extensive trawling and physical activities. The obtained ratio profiles showed excess of (234)Th relative to (238)U in the BNL of the sampling area during summer, caused by the dissolved fraction of (234)Th. During autumn, the situation was different with large (234)Th deficit throughout the water column leading to large export fluxes of particles from the water column. Finally, during winter the ratios showed that predominant phenomenon in the area was likely resuspension of bottom sediments. The resuspension signature was additionally evaluated by total suspended matter (TSM) inventories in the BNL. Despite the intense resuspension, small scavenging of dissolved (234)Th was recorded in the BNL resulting in high residence times of dissolved (234)Th. A 1 order of magnitude difference between dissolved and particulate (234)Th residence times was observed indicating that scavenging from dissolved to particulate (234)Th could be highly variable and, as a result, the Saronikos Gulf is a highly dynamic environment, in terms of temporal and spatial particle uptake and removal. Comparing these values to literature ones consistent results were obtained. The possibility of sediment resuspension in the BNL during winter was amplified by the bloom of phytoplankton resulting in even decreased residence times of particulate (234)Th (average values). In contrast, the respective residence times of the dissolved fraction of (234)Th in the BNL were higher showing a maximum in winter at the stations where resuspension concluded. Nevertheless, (234)Th cycling in the area is not controlled by TSM, probably due to the presence of colloids, which could play an essential role in (234)Th scavenging.

Validation of Hansen-Roach library for highly enriched uranium metal systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wenz, T.R.; Busch, R.D.

The Hansen-Roach 16-group cross-section library has been validated for use in pure uranium metal systems by modeling the Godiva critical assembly using the neutronics transport theory code ONEDANT to perform effective multiplication factor (k{sub eff}) calculations. The cross-section library used contains data for 118 isotopes (34 unique elements), including the revised cross sections for {sup 235}U and {sup 238}U. The Godiva critical assembly is a 17.4-cm sphere composed of 93.7 wt% {sup 235}U, 1.0 wt% {sup 234}U, and 5.3 wt% {sup 238}U with an effective homogeneous density of 18.7 g/cm{sup 3}.

Uranium isotopes in groundwater occurring at Amazonas State, Brazil.

PubMed

da Silva, Márcio Luiz; Bonotto, Daniel Marcos

2015-03-01

This paper reports the behavior of the dissolved U-isotopes (238)U and (234)U in groundwater providing from 15 cities in Amazonas State, Brazil. The isotope dilution technique accompanied by alpha spectrometry were utilized for acquiring the U content and (234)U/(238)U activity ratio (AR) data, 0.01-1.4µgL(-1) and 1.0-3.5, respectively. These results suggest that the water is circulating in a reducing environment and leaching strata containing minerals with low uranium concentration. A tendency to increasing ARs values following the groundwater flow direction is identified in Manaus city. The AR also increases according to the SW-NE directions: Uarini→Tefé; Manacapuru→Manaus; Presidente Figueiredo→São Sebastião do Uatumã; and Boa Vista do Ramos→Parintins. Such trends are possibly related to several factors, among them the increasing acid character of the waters. The waters analyzed are used for human consumption and the highest dissolved U content is much lower than the maximum established by the World Health Organization. Therefore, in view of this radiological parameter they can be used for drinking purposes. Copyright © 2014 Elsevier Ltd. All rights reserved.

In-situ measurements of U-series nuclides by electron microprobe on zircons and monazites from Gandak river sediments

NASA Astrophysics Data System (ADS)

Bosia, C.; Deloule, E.; France-Lanord, C.; Chabaux, F.

2015-12-01

Determination of sediment transfer time during transport in the alluvial plains is a critical issue to correctly understand the relationship between climate, tectonics and Earth surface evolution. The residence time of river sediments may be constrained by analyzing the U series nuclides fractionations (e.g. [1] and [2]), which are created during water rock interactions by the ejection of the daughter nuclides of the grain (α-recoil) and the preferential mobilization of nuclides in decay damaged crystal structure. However, recent studies on sediments from the Gandak river, one of the main Ganga tributary, highlighted the difficulties to obtain reproducible data on bulk sediments, due to the nuggets distribution of U-Th enriched minor minerals in the samples (Bosia et al., unpublished data). We therefore decided to analyze the U and Th isotopic systematic at a grain-scale for Himalayan sediments from the Gandak river. This has been tested by performing in situ depth profiles of 238U-234U-230Th and 232Th on zircons and monazites (50-250 μm) by Secondary Ion Mass Spectrometry (SIMS) at the CRPG, Nancy, France. The first results point the occurrence of 238U-234U-230Th disequilibria in the outermost parts of both monazite and zircon minerals with a return to the equilibrium state in the core of the grains. The relative U and Th enrichment is however slightly different depending on considered minerals, suggesting possible adsorption processes of 230-Th. Coupled to a simple model of U and Th mobility during water-mineral interactions, these data should help to constrain the origin of 238U-234U-230Th disequilibria in these minerals. Moreover, the results of the study should be relevant to discuss the potential of this approach to constrain the residence time of zircons and monazites in the Gandak alluvial plain. [1] Chabaux et al., 2012, C. R. Geoscience, 344 (11-12): 688-703; [2] Granet et al., 2007, Earth and Planet. Sci. Lett., 261 (3-4): 389-406.

Residual β activity of particulate (234)Th as a novel proxy for tracking sediment resuspension in the ocean.

PubMed

Lin, Wuhui; Chen, Liqi; Zeng, Shi; Li, Tao; Wang, Yinghui; Yu, Kefu

2016-06-02

Sediment resuspension occurs in the global ocean, which greatly affects material exchange between the sediment and the overlying seawater. The behaviours of carbon, nutrients, heavy metals, and other pollutants at the sediment-seawater boundary will further link to climate change, eutrophication, and marine pollution. Residual β activity of particulate (234)Th (RAP234) is used as a novel proxy to track sediment resuspension in different marine environments, including the western Arctic Ocean, the South China Sea, and the Southern Ocean. Sediment resuspension identified by high activity of RAP234 is supported by different lines of evidence including seawater turbidity, residence time of total (234)Th, Goldschmidt's classification, and ratio of RAP234 to particulate organic carbon. A conceptual model is proposed to elucidate the mechanism for RAP234 with dominant contributions from (234)Th-(238)U and (212)Bi-(228)Th. The 'slope assumption' for RAP234 indicated increasing intensity of sediment resuspension from spring to autumn under the influence of the East Asian monsoon system. RAP234 can shed new light on (234)Th-based particle dynamics and should benefit the interpretation of historical (234)Th-(238)U database. RAP234 resembles lithophile elements and has broad implications for investigating particle dynamics in the estuary-shelf-slope-ocean continuum and linkage of the atmosphere-ocean-sediment system.

Residual β activity of particulate 234Th as a novel proxy for tracking sediment resuspension in the ocean

PubMed Central

Lin, Wuhui; Chen, Liqi; Zeng, Shi; Li, Tao; Wang, Yinghui; Yu, Kefu

2016-01-01

Sediment resuspension occurs in the global ocean, which greatly affects material exchange between the sediment and the overlying seawater. The behaviours of carbon, nutrients, heavy metals, and other pollutants at the sediment-seawater boundary will further link to climate change, eutrophication, and marine pollution. Residual β activity of particulate 234Th (RAP234) is used as a novel proxy to track sediment resuspension in different marine environments, including the western Arctic Ocean, the South China Sea, and the Southern Ocean. Sediment resuspension identified by high activity of RAP234 is supported by different lines of evidence including seawater turbidity, residence time of total 234Th, Goldschmidt’s classification, and ratio of RAP234 to particulate organic carbon. A conceptual model is proposed to elucidate the mechanism for RAP234 with dominant contributions from 234Th-238U and 212Bi-228Th. The ‘slope assumption’ for RAP234 indicated increasing intensity of sediment resuspension from spring to autumn under the influence of the East Asian monsoon system. RAP234 can shed new light on 234Th-based particle dynamics and should benefit the interpretation of historical 234Th-238U database. RAP234 resembles lithophile elements and has broad implications for investigating particle dynamics in the estuary-shelf-slope-ocean continuum and linkage of the atmosphere-ocean-sediment system. PMID:27252085

Seasonal variations of natural radionuclides, minor and trace elements in lake sediments and water in a lignite mining area of North-Western Greece.

PubMed

Noli, Fotini; Tsamos, Panagiotis

2018-05-01

The radiological and chemical pollution of a cluster of four lakes in a lignite mining area of North-Western Greece was investigated using a variety of analytical techniques. Alpha spectrometry was applied to measure the activity concentrations of the uranium radioisotopes (U-234, U-235, and U-238) in waters. The mass activities of U-238, Th-232, and K-40 in sediments were measured by high-resolution gamma spectrometry. Furthermore, the determination of the minor and trace elements was carried out by instrumental neutron activation analysis (INAA) in both water and sediments samples, respectively. Pollution levels were also evaluated by calculating enrichment factors (EFs), contamination factors (CFs) and pollution load index (PLI). The data were discussed taking into account several parameters such as the distance from the pollution source, temperature, and location and showed that the environmental impact in this region could not be considered as negligible. The deviation of the isotopic ratio of U-234/U-238 from the equilibrium value indicated waters with intensive dissolution of uranium. The activity values in both waters and sediments found to be low in cool periods and increased in warm periods. Moreover, the concentrations of the elements U, Zn, and Fe were raised in water samples indicating possible pollution as well as the CFs and PLI denoted accumulation in the sediments and moderate to severe contamination for Zn and Cr in some cases.

Potential human health risk by 234,238U and 210Po due to consumption of fish from the "Luis L. Leon" reservoir (Northern Mexico)

NASA Astrophysics Data System (ADS)

Luna-Porres, M. Y.; Rodríguez-Villa, M. A.; Herrera-Peraza, E.; Cabral-Lares, M.; Renteria-Villalobos, M.; Montero-Cabrera, M. E.

2014-07-01

The Conchos River is one of the most important in northern Mexico and the main surface waterway in the arid state of Chihuahua. The Luis L. Leon dam produces the Luis L. Leon Reservoir, which is the last major reservoir before the Conchos River enters the Rio Grande at the Texas-Chihuahua border. Activity concentrations (AC) of 234,238U and 210Po in fillet and liver of three stocked fish species (Lepomis cyanellus, Cyprinus carpio and Ictalurus furcatus), as well as in water from the Luis L. Leon reservoir were determined. 238U and 234U ACs in fillet samples showed values of 0.007-0.014 and 0.01-0.02 Bq kg-1 wet weight (ww), respectively. Liver samples for Lepomis cyanellus, Cyprinus carpio and Ictalurus furcatus species, present 210Po AC of 1.16-3.26 0.70-1.13 and 0.93-1.37 Bqṡkg-1 ww. The elemental Bioaccumulation Factor (BAF) for fish tissues respect to their concentrations in water was determined. Lepomis cyanellus species showed the highest BAF for total uranium in fillet, with value 1.5. The annual effective dose for uranium in adults by fish consumption in this work ranged from 4.46×10-3 to 3.68×10-2 μSvṡyear-1. The difference in concentrations of uranium in fillet among the studied species is likely primarily due to their differences in diet and habitat.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

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 inmore » 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.« less

Study of uranium oxidation states in geological material.

PubMed

Pidchenko, I; Salminen-Paatero, S; Rothe, J; Suksi, J

2013-10-01

A wet chemical method to determine uranium (U) oxidation states in geological material has been developed and tested. The problem faced in oxidation state determinations with wet chemical methods is that U redox state may change when extracted from the sample material, thereby leading to erroneous results. In order to quantify and monitor U redox behavior during the acidic extraction in the procedure, an analysis of added isotopic redox tracers, (236)U(VI) and (232)U(IV), and of variations in natural uranium isotope ratio ((234)U/(238)U) of indigenous U(IV) and U(VI) fractions was performed. Two sample materials with varying redox activity, U bearing rock and U-rich clayey lignite sediment, were used for the tests. The Fe(II)/Fe(III) redox-pair of the mineral phases was postulated as a potentially disturbing redox agent. The impact of Fe(III) on U was studied by reducing Fe(III) with ascorbic acid, which was added to the extraction solution. We observed that ascorbic acid protected most of the U from oxidation. The measured (234)U/(238)U ratio in U(IV) and U(VI) fractions in the sediment samples provided a unique tool to quantify U oxidation caused by Fe(III). Annealing (sample heating) to temperatures above 500 °C was supposed to heal ionizing radiation induced defects in the material that can disturb U redox state during extraction. Good agreement between two independent methods was obtained for DL-1a material: an average 38% of U(IV) determined by redox tracer corrected wet chemistry and 45% for XANES. Copyright © 2013 Elsevier Ltd. All rights reserved.

Distribution of radioactive isotopes in rock and ore of Arkhangelskaya pipe from the Arkhangelsk diamond province

NASA Astrophysics Data System (ADS)

Kiselev, G. P.; Yakovlev, E. Yu.; Druzhinin, S. V.; Galkin, A. S.

2017-09-01

The contents of radioactive elements and the uranium isotopic composition of kimberlite in the Arkhangelskaya pipe at the M.V. Lomonosov deposit and of nearby country rocks have been studied. A surplus of 234U isotope has been established in rocks from the near-pipe space. The high γ = 234U/238U ratio is controlled by the geological structure of the near-pipe space. A nonequilibrium uranium halo reaches two pipe diameters in size and can be regarded as a local ore guide for kimberlite discovery. The rocks in the nearpipe space are also characterized by elevated or anomalous U, Th, and K contents with respect to the background.

Radiation protection and radioactive scales in oil and gas production.

PubMed

Testa, C; Desideri, D; Meli, M A; Roselli, C; Bassignani, A; Colombo, G; Fantoni, R F

1994-07-01

Low specific-activity scales consisting of alkaline earth metal carbonates and sulfates are often present in some gaseous and liquid hydrocarbon plants. These scales contain a certain concentration of radium, uranium, and thorium which can cause a risk of gamma irradiation and internal radiocontamination when they must be mechanically removed. The gamma dose rates and the 238U, 232Th, 226Ra concentrations were determined in sludges, scales, and waters of some gas and oil hydrocarbon plants located in Italy, Congo, and Tunisia. 238U and 232Th concentrations were were low. The isotopes 238U and 234U resulted in radioactive equilibrium, while 232Th and 228Th were not always equilibrium. A rough correlation was found between the gamma dose rate and the 226Ra concentration. Some considerations and conclusions about radiation protection problems are pointed out.

Uranium-series disequilibrium in tuffs from Yucca Mountain, Nevada, as evidence of pore-fluid flow over the last million years

USGS Publications Warehouse

Gascoyne, M.; Miller, N.H.; Neymark, L.A.

2002-01-01

Samples of tuff from boreholes drilled into fault zones in the Exploratory Studies Facility (ESF) and relatively unfractured rock of the Cross Drift tunnels, at Yucca Mountain, Nevada, have been analysed by U-series methods. This work is part of a project to verify the finding of fast flow-paths through the tuff to ESF level, indicated by the presence of 'bomb' 36Cl in pore fluids. Secular radioactive equilibrium in the U decay series, (i.e. when the radioactivity ratios 234U/238U, 230Th/234U and 226Ra/230Th all equal 1.00) might be expected if the tuff samples have not experienced radionuclide loss due to rock-water interaction occurring within the last million years. However, most fractured and unfractured samples were found to have a small deficiency of 234U (weighted mean 234U/238U=0.95??0.01) and a small excess of 230Th (weighted mean 230Th/234U 1.10??0.02). The 226Ra/230Th ratios are close to secular equilibrium (weighted mean = 0.94??0.07). These data indicate that 234U has been removed from the rock samples in the last ???350 ka, probably by pore fluids. Within the precision of the measurement, it would appear that 226Ra has not been mobilized and removed from the tuff, although there may be some localised 226Ra redistribution as suggested by a few ratio values that are significantly different from 1.0. Because both fractured and unfractured tuffs show approximately the same deficiency of 234U, this indicates that pore fluids are moving equally through fractured and unfractured rock, More importantly, fractured rock appears not to be a dominant pathway for groundwater flow (otherwise the ratio would be more strongly affected and the Th and Ra isotopic ratios would likely also show disequilibrium). Application of a simple mass-balance model suggests that surface infiltration rate is over an order of magnitude greater than the rate indicated by other infiltration models and that residence time of pore fluids at ESF level is about 400 a. Processes of U sorption, precipitation and re-solution are believed to be occurring and would account for these anomalous results but have not been included in the model. Despite the difficulties, the U-series data suggest that fractured rock, specifically the Sundance and Drill Hole Wash faults, are not preferred flow paths for groundwater flowing through the Topopah Spring tuff and, by implication, rapid-flow, within 50 a, from the surface to the level of the ESF is improbable. ?? 2002 Elsevier Science Ltd. All rights reserved.

Natural radionuclides in plants, soils and sediments affected by U-rich coal mining activities in Brazil.

PubMed

Galhardi, Juliana Aparecida; García-Tenorio, Rafael; Bonotto, Daniel Marcos; Díaz Francés, Inmaculada; Motta, João Gabriel

2017-10-01

Mining activities can increase the mobility of metals by accelerating the dissolution and leaching of minerals from the rocks and tailing piles to the environment and, consequently, their availability for plants and subsequent transfer to the food chain. The weathering of minerals and the disposal of coal waste in tailing piles can accelerate the generation of acid mine drainage (AMD), which is responsible for the higher dissolution of metals in mining areas. In this context, the behavior of U, Th and K in soils and sediment, and the transfer factor (TF) of 238 U, 234 U and 210 Po for soybean, wheat, pine and eucalyptus cultivated around a coal mine in southern Brazil was evaluated. Alpha and gamma spectrometry were used for the measurements of the activity concentration of the radioelements. 210 Po was the radionuclide that is most accumulated in the plants, especially in the leaves. When comparing the plant species, pine showed the highest TF values for 234 U (0.311 ± 0.420) for leaves, while eucalyptus showed the highest TF for 238 U (0.344 ± 0.414) for leaves. In general, TF were higher for the leaves of soybean and wheat when compared to the grains, and grains of wheat showed higher TF for 210 Po and 238 U than grains of soybean. Deviations from the natural U isotopic ratio were recorded at all investigated areas, indicating possible industrial and mining sources of U for the vegetables. A safety assessment of transport routes and accumulation of radionuclides in soils with a potential for cultivation is important, mainly in tropical areas contaminated with solid waste and effluents from mines and industry. Copyright © 2017 Elsevier Ltd. All rights reserved.

Investigation of uranium geochemistry along groundwater flow path in the Continental Intercalaire aquifer (Southern Tunisia).

PubMed

Dhaoui, Z; Chkir, N; Zouari, K; Ammar, F Hadj; Agoune, A

2016-06-01

Environmental tracers ((2)H, (18)O, isotopes of Uranium) and geochemical processes occurring within groundwaters from the Continental Intercalaire (CI) in Southern Tunisia were used to understand the hydrodynamics and the recharge conditions of this aquifer. This study investigates the chemical and isotopic compositions of the CI groundwater. The water types are dominated by Na(+), SO4(2-), Cl(-) throughout most of the basin with a general increase in total dissolved solids from the Saharan Platform margins towards the Chotts region. Large scale groundwater flow paths are toward the Chotts region. The stable isotopes composition of the analyzed groundwater ranges from -8.8 to -6‰ vs V-SMOW for δ(18)O and from -67 to -40‰ vs V-SMOW for δ(2)H. The relatively enriched stable isotopes contents suggest the contribution of the Dahar sandstones outcrops in the current recharge of the CI aquifer in an arid context. However, the most depleted values in heavy isotopes indicate a paleorecharge of the aquifer under wetter conditions revealing a long residence time of groundwaters. The results from water samples using alpha spectrometry method indicate a range in (238)U concentrations and (234)U/(238)U activity ratios (AR) of 0.044-1.285 μg kg(-1) and 1.2 to 8.84 respectively. The geochemistry of uranium isotopes in groundwater is controlled by many factors, essentially, the influence of water rock interactions, the preferential dissolution of (234)U relative to (238)U due to alpha recoil and the mixing processes between different waters with distinct AR as well as (238)U concentrations. Copyright © 2016 Elsevier Ltd. All rights reserved.

Rates of carbonate soil evolution from carbon, U- and Th-series isotope studies: Example of the Astian sands (SE France)

NASA Astrophysics Data System (ADS)

Barbecot, Florent; Ghaleb, Bassam; Hillaire-Marcel, Claude

2015-04-01

In carbonate rich soils, C-isotopes (14C, 13C) and carbonate mass budget may inform on centennial to millennial time scale dissolution/precipitation processes and weathering rates, whereas disequilibria between in the U- and Th-decay series provide tools to document high- (228Ra-228Th-210Pb) to low- (234U, 230Th, 231Pa, 226Ra) geochemical processes rate, covering annual to ~ 1Ma time scales, governing both carbonate and silicate soil fractions. Because lithology constitutes a boundary condition, we intend to illustrate the behavior of such isotopes in soils developed over Astian sands formation (up to ~ 30% carbonate) from the Béziers area (SE France). A >20 m thick unsaturated zone was sampled firstly along a naturally exposed section, then in a cored sequence. Geochemical and mineralogical analyses, including stable isotopes and 14C-measurements, were complemented with 228U, 234U, 230Th, 226Ra, 210Pb and 228Th, 232Th measurements. Whereas the upper 7 m depict geochemical and isotopic features forced by dissolution/precipitation processes leading to variable radioactive disequilibria, but overall deficits in more soluble elements of the decay series, the lower part of the sequence shows strong excesses in 234U and 230Th over parent isotopes (i.e., 238U and 234U, respectively). These features might have been interpreted as the result of successive phases of U-loss and gains. However, 226Ra and 230Th are in near-equilibrium, thus leading to conclude at a more likely slow enrichment process in both 234Th(234U) and 230Th, which we link to dissolved U-decay during groundwater recharge events. In addition, 210Pb deficits (vs parent 226Ra) are observed down to 12 m along the natural outcropping section and below the top-soil 210Pb-excess in the cored sequence, due to gaseous 222Rn-diffusion over the cliff outcrop. Based on C-isotope and chemical analysis, reaction rates at 14C-time scale are distinct from those estimates at the short- or long-lived U-series isotopes, but provide a specific insight into carbonate budgets when confronted with data on dissolved and gaseous phases as well as on solid matter, and possibly best integrate the overall soil behavior through time. It is concluded from this example that if first order estimates of long-term geochemical fluxes in soils can be obtained from disequilibria in the 238U-234U-230Th sequence or from C-isotope data. While insights into recent to "Anthropocene" processes require information on the shorter-lived isotopes of the U and Th series, adding specific information on physical and chemical erosion budgets from 232Th data. As also illustrated in the present example, a robust assessment of overall chemical and physical erosion rates must be based on measurements in cored sequences away from natural or recent man-made cuts.

EC comparison on the determination of 226Ra, 228Ra, 234U and 238U in water among European monitoring laboratories.

PubMed

Wätjen, U; Benedik, L; Spasova, Y; Vasile, M; Altzitzoglou, T; Beyermann, M

2010-01-01

In anticipation of new European requirements for monitoring radioactivity concentration in drinking water, IRMM organized an interlaboratory comparison on the determination of low levels of activity concentrations (about 10-100 mBq L(-1)) of the naturally occurring radionuclides (226)Ra, (228)Ra, (234)U and (238)U in three commercially available mineral waters. Using two or three different methods with traceability to the International System of Reference (SIR), the reference values of the water samples were determined prior to the proficiency test within combined standard uncertainties of the order of 3%-10%. An overview of radiochemical separation and measurement methods used by the 45 participating laboratories are given. The results of the participants are evaluated versus the reference values. Several of the participants' results deviate by more than a factor of two from the reference values, in particular for the radium isotopes. Such erroneous analysis results may lead to a crucial omission of remedial actions on drinking water supplies or to economic loss by an unjustified action. Copyright 2009 Elsevier Ltd. All rights reserved.

DETERMINATION AND DOSE CONTRIBUTION OF URANIUM ISOTOPES AND 210Po ACTIVITY CONCENTRATIONS OF NATURAL SPRING WATERS IN THE PROVINCE OF GRANADA, SPAIN.

PubMed

Milena-Pérez, A; Piñero-García, F; Expósito-Suárez, V M; Mantero, J; Benavente, J; Ferro-García, M A

2018-03-01

The activity concentrations of alpha-emitters comprising isotopes of uranium (238, 234, 235U) and polonium (210Po) were measured using alpha-particle spectrometry in natural spring waters in the province of Granada, Spain. These water are consumed by the population of the zone who live in villages. This is almost half of the population of the whole region. Mean values of activity concentrations found are 42.61 ± 2.66; 49.55 ± 3.03; 1.64 ± 0.28 and 1.74 ± 0.15 mBq L-1 for 238U, 234U, 235U and 210Po, respectively. Finally, the radiological impact of the analysed waters has been determined, in terms of the estimation of the committed annual effective dose due to the ingestion of the water. The assessment has been carried out for five age groups with the aim to cover all the population. The calculated annual effective doses are observed to be below the prescribed dose limit of 100 μSv y-1 recommended by WHO.

Chemistry of uranium, thorium, and radium isotopes in the Ganga-Brahmaputra river system: Weathering processes and fluxes to the Bay of Bengal

NASA Astrophysics Data System (ADS)

Sarin, M. M.; Krishnaswami, S.; somayajulu, B. L. K.; Moore, W. S.

1990-05-01

The most comprehensive data set on uranium, thorium, and radium isotopes in the Ganga-Brahmaputra, one of the major river systems of the world, is reported here. The dissolved 238U concentration in these river waters ranges between 0.44 and 8.32 μ/1, and it exhibits a positive correlation with major cations (Na + K + Mg + Ca). The 238U /∑Cations ratio in waters is very similar to that measured in the suspended sediments, indicating congruent weathering of uranium and major cations. The regional variations observed in the [ 234U /238U ] activity ratio are consistent with the lithology of the drainage basins. The lowland tributaries (Chambal, Betwa, Ken, and Son), draining through the igneous and metamorphic rocks of the Deccan Traps and the Vindhyan-Bundelkhand Plateau, have [ 234U /238U ] ratio in the range 1.16 to 1.84. This range is significantly higher than the near equilibrium ratio (~1.05) observed in the highland rivers which drain through sedimentary terrains. The dissolved 226Ra concentration ranges between 0.03 and 0.22 dpm/1. The striking feature of the radium isotopes data is the distinct difference in the 228Ra and 226Ra abundances between the highland and lowland rivers. The lowland waters are enriched in 228Ra while the highland waters contain more 226Ra. This difference mainly results from the differences in their weathering regimes. The discharge-weighted mean concentration of dissolved 238U in the Ganga (at Patna) and in the Brahmaputra (at Goalpara) are 1.81 and 0.63 μ/1, respectively. The Ganga-Brahmaputra river system constitutes the major source of dissolved uranium to the Bay of Bengal. These rivers transport annually about 1000 tons of uranium to their estuaries, about 10% of the estimated global supply of dissolved uranium to the oceans via rivers. The transport of uranium by these rivers far exceeds that of the Amazon, although their water discharge is only about 20% of that of the Amazon. The high intensity of weathering of uranium in the Ganga-Brahmapura River system can also be deduced from the [ 232Th /238U ] and [ 230Th /238U ] activity ratios measured in the suspended sediments. 230Th is enriched by about 19% in the suspended sediments relative to its parent 238U. The flux of excess 230Th supplied to the Bay of Bengal via these river sediments is 980 × 10 12 dpm/a, about six times more than its in situ production from seawater in the entire Bay of Bengal.

Early-Mid Holocene climatic variations in Tasmania, Australia: multi-proxy records in a stalagmite from Lynds Cave

NASA Astrophysics Data System (ADS)

Xia, Qikai; Zhao, Jian-xin; Collerson, K. D.

2001-12-01

Mass spectrometric uranium-series dating and C-O isotopic analysis of a stalagmite from Lynds Cave, northern Tasmania, Australia provide a high-resolution record of regional climate change between 5100 and 9200 yr before present (BP). Combined δ18O, δ13C, growth rate, initial 234U/238U and physical property (color, transparency and porosity) records allow recognition of seven climatic stages: Stage I (>9080 yr BP) - a relatively dry period at the beginning of stalagmite growth evidenced by elevated 234U/238U; Stage II (9080-8600 yr BP) - a period of unstable climate characterized by high-frequency variability in temperature and bio-productivity; Stage III (8600-8000 yr BP) - a period of stable and moderate precipitation and stable and high bio-productivity, with a continuously rising temperature; Stage IV (8000-7400 yr BP) - the warmest period with high evaporation and low effective precipitation (rainfall less evaporation); Stage V (7400-7000 yr BP) - the wettest period with highest stalagmite growth and enhanced but unstable bio-productivity; Stage VI (7000-6600 yr BP) - a period with a significantly reduced precipitation and bio-productivity without noticeable change in temperature; Stage VII (6600-5100 yr BP) - a period of lowest temperature and precipitation marking a significant climatic deterioration. Overall, the records suggest that the warmest climate occurred between 8000 and 7400 yr BP, followed by a wettest period between 7400 and 7000 yr BP. These are broadly correlated with the so-called 'Mid Holocene optimum' previously proposed using pollen and lake level records. However, the timing and resolution of the speleothem record from Lynds Cave are significantly higher than in both the pollen and lake level records. This allows us to correlate the abrupt change in physical property, δ18O, δ13C, growth rate, and initial 234U/238U of the stalagmite at ˜8000 yr BP with a global climatic event at Early-Mid Holocene transition.

Natural and man-made radioactivity in soils and plants around the research reactor of Inshass.

PubMed

Higgy, R H; Pimpl, M

1998-12-01

The specific radioactivities of the U-series, 232Th, 137Cs and 40K were measured in soil samples around the Inshass reactor in Cairo, using a gamma-ray spectrometer with a HpGe detector. The alpha activity of 238U, 234U and 235U was measured in the same soil samples by surface barrier detectors after radiochemical separation and the obtained results were compared with the specific activities determined by gamma-measurements. The alpha-activity of 238Pu, 239+240Pu, 241Am, 242Cm and 244Cm was measured after radiochemical separation by surface barrier detectors for both soil and plant samples. Then beta-activity of 241Pu was measured using liquid scintillation spectrometry.

Polonium (²¹⁰Po), uranium (²³⁴U, ²³⁸U) isotopes and trace metals in mosses from Sobieszewo Island, northern Poland.

PubMed

Boryło, Alicja; Nowicki, Waldemar; Olszewski, Grzegorz; Skwarzec, Bogdan

2012-01-01

The activity of polonium (210)Po and uranium (234)U, (238)U radionuclides, as well as trace metals in mosses, collected from Sobieszewo Island area (northern Poland), were determined using the alpha spectrometry, AAS (atomic absorption spectrometry) and OES-ICP (atomic emission spectrometry with inductively coupled plasma). The concentrations of mercury (directly from the solid sample) were determined by the cold vapor technique of CV AAS. The obtained results revealed that the concentrations of (210)Po, (234)U, and (238)U in the two analyzed kinds of mosses: schrebers big red stem moss (Pleurozium schreberi) and broom moss (Dicranum scoparium) were similar. The higher polonium concentrations were found in broom moss (Dicranum scoparium), but uranium concentrations were relatively low for both species of analyzed mosses. Among the analyzed trace metals the highest concentration in mosses was recorded for iron, while the lowest for nickel, cadmium and mercury. The obtained studies showed that the sources of polonium and uranium isotopes, as well as trace metals in analyzed mosses are air city contaminations transported from Gdańsk and from existing in the vicinity the phosphogypsum waste heap in Wiślinka (near Gdańsk).

Fertilizer-derived uranium and sulfur in rangeland soil and runoff: A case study in central Florida

USGS Publications Warehouse

Zielinski, R.A.; Orem, W.H.; Simmons, K.R.; Bohlen, P.J.

2006-01-01

Fertilizer applications to rangeland and pastures in central Florida have potential impact on the nutrient-sensitive ecosystems of Lake Okeechobee and the Northern Everglades. To investigate the effects of fertilizer applications, three soil profiles from variably managed and improved rangeland, and four samples of surface runoff from both fertilized and unfertilized pasture were collected. In addition to determining nutrient concentrations, isotopic analyses of uranium (U) and sulfur (S) were performed to provide isotopic evidence for U derived from historically applied phosphate (P)-bearing fertilizer ( 234 U 238U activity ratio =1.0 ?? 0.05), and Sderived from recently applied ammonium sulfate fertilizer(??34 S=3.5permil).The distribution and mobility of fertilizer-derived U in these samples is considered to be analogous to that of fertilizer-derived phosphate.Variations of U concentrations and 234 U/238 U activity ratios in soils indicate contribution of fertilizer-derived U in the upper portions of the fertilized soil (15-}34 percent of total U). The U isotope data for runoff from the fertilized field also are consistent with some contribution from fertilizer-derived U. Parallel investigations of S showed no consistent chemical or isotopic evidence for significant fertilizer-derived sulfate in rangeland soil or runoff. Relatively abundant and isotopically variable S present in the local environment hinders detection of fertilizer-derived sulfate. The results indicate a continuing slow-release of fertilizer-derived U and, by inference, P, to the P-sensitive ecosystem, and a relatively rapid release of sulfate of possible natural origin. ?? Springer 2006.

Regolith formation rate from U-series nuclides: Implications from the study of a spheroidal weathering profile in the Rio Icacos watershed (Puerto Rico)

NASA Astrophysics Data System (ADS)

Chabaux, F.; Blaes, E.; Stille, P.; di Chiara Roupert, R.; Pelt, E.; Dosseto, A.; Ma, L.; Buss, H. L.; Brantley, S. L.

2013-01-01

A 2 m-thick spheroidal weathering profile, developed on a quartz diorite in the Rio Icacos watershed (Luquillo Mountains, eastern Puerto Rico), was analyzed for major and trace element concentrations, Sr and Nd isotopic ratios and U-series nuclides (238U-234U-230Th-226Ra). In this profile a 40 cm thick soil horizon is overlying a 150 cm thick saprolite which is separated from the basal corestone by a ˜40 cm thick rindlet zone. The Sr and Nd isotopic variations along the whole profile imply that, in addition to geochemical fractionations associated to water-rock interactions, the geochemical budget of the profile is influenced by a significant accretion of atmospheric dusts. The mineralogical and geochemical variations along the profile also confirm that the weathering front does not progress continuously from the top to the base of the profile. The upper part of the profile is probably associated with a different weathering system (lateral weathering of upper corestones) than the lower part, which consists of the basal corestone, the associated rindlet system and the saprolite in contact with these rindlets. Consequently, the determination of weathering rates from 238U-234U-230Th-226Ra disequilibrium in a series of samples collected along a vertical depth profile can only be attempted for samples collected in the lower part of the profile, i.e. the rindlet zone and the lower saprolite. Similar propagation rates were derived for the rindlet system and the saprolite by using classical models involving loss and gain processes for all nuclides to interpret the variation of U-series nuclides in the rindlet-saprolite subsystem. The consistency of these weathering rates with average weathering and erosion rates derived via other methods for the whole watershed provides a new and independent argument that, in the Rio Icacos watershed, the weathering system has reached a geomorphologic steady-state. Our study also indicates that even in environments with differential weathering, such as observed for the Puerto Rico site, the radioactive disequilibrium between the nuclides of a single radioactive series (here 238U-234U-230Th-226Ra) can still be interpreted in terms of a simplified scenario of congruent weathering. Incidentally, the U-Th-Ra disequilibrium in the corestone samples confirms that the outermost part of the corestone is already weathered.

234Th: 238U disequilibrium as an indicator of sediment resuspension in Thermaikos Gulf, northwestern Aegean Sea

NASA Astrophysics Data System (ADS)

Muir, G. K. P.; Pates, J. M.; Karageorgis, A. P.; Kaberi, H.

2005-12-01

234Th: 238U disequilibria have been used extensively as tracers of particle dynamics in marine environments. 234Th ( t1/2=24.1 days) can be used as "proxy" for particle reactive pollutants, due to their similar rapid rate of scavenging onto particles and subsequent removal from the water column, to the sediments. Radioactive disequilibrium can be exploited to determine the rates and time-scales of processes occurring over days to months; in this instance the residence times of dissolved and particulate species with the benthic nepheloid layer (BNL). Three sampling cruises were undertaken in Thermaikos Gulf (NW Aegean Sea) during contrasting periods, to examine the impact of natural and anthropogenic activity on sediment resuspension. September and October 2001 represented background and trawling periods, respectively; January 2002 represented a mixed period, of trawling and storms. Dissolved 234Th is scavenged actively at the BNL, in the presence of suspended particulate material (SPM), with a mean residence time of 16 days. There is a weak inverse correlation between dissolved 234Th residence time and SPM concentration in the BNL, with the shortest residence times occurring during October 2001. No relationship was observed between particulate 234Th activities and SPM concentrations, indicating that particles are rapidly removed from the system, either by sinking or advection. The mean particulate 234Th residence time is 5 days.

Air and radon pathways screenings methodologies for the next revision of the E-area PA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dyer, J. A.

The strategic plan for the next E-Area Low-Level Waste Facility Performance Assessment includes recommended changes to the screening criteria used to reduce the number of radioisotopes that are to be considered in the air and radon pathways incorporated into the GoldSim® atmospheric release model (ARM). For the air pathway, a revised screening methodology was developed based on refinement of previous E-Area PA screening approaches and consideration of the strategic plan recommendations. The revised methodology has three sequential screening steps for each radioisotope: (1) volatility test using the Periodic Table of the Elements, (2) stability test based on half-life, and (3)more » stability test based on volatility as measured by the Henry’s Law constant for the assumed dominant gaseous species or vapor pressure in the case of tritiated water. Of the 1252 radioisotopes listed in the International Commission on Radiological Protection Publication 107, only the 10 that satisfied all three steps of the revised screening methodology will be included in the ARM. They are: Ar-37, Ar-39, Ar-42, C-14, H-3, Hg-194, Hg-203, Kr-81, Kr-85, and Xe-127. For the radon pathway, a revised screening methodology was developed that also has three sequential steps: (1) identify all decay chains that terminate at Rn-222, (2) screen out parents that decay through U-238 because of its 4.5-billion-year primordial half-life, and (3) eliminate remaining parents whose half-life is shorter than one day. Of the 86 possible decay chains leading to Rn-222, six decay chains consist of 15 unique radioisotopes that will be incorporated into the ARM. The 15 radioisotopes are: U-238, Th-234, Pa-234m, Pu-238, U-234, Th-230, Ra-226, Cf-246, Cm-242, Am-242m, Am-242, Np-238, Np-234, Pa-230, and Rn-222.« less

Depleted and enriched uranium exposure quantified in former factory workers and local residents of NL Industries, Colonie, NY USA.

PubMed

Arnason, John G; Pellegri, Christine N; Moore, June L; Lewis-Michl, Elizabeth L; Parsons, Patrick J

2016-10-01

Between 1958 and 1982, NL Industries manufactured components of enriched (EU) and depleted uranium (DU) at a factory in Colonie NY, USA. More than 5 metric tons of DU was deposited as microscopic DU oxide particles on the plant site and surrounding residential community. A prior study involving a small number of individuals (n=23) indicated some residents were exposed to DU and former workers to both DU and EU, most probably through inhalation of aerosol particles. Our aim was to measure total uranium [U] and the uranium isotope ratios: (234)U/(238)U; (235)U/(238)U; and (236)U/(238)U, in the urine of a cohort of former workers and nearby residents of the NLI factory, to characterize individual exposure to natural uranium (NU), DU, and EU more than 3 decades after production ceased. We conducted a biomonitoring study in a larger cohort of 32 former workers and 99 residents, who may have been exposed during its period of operation, by measuring Total U, NU, DU, and EU in urine using Sector Field Inductively Coupled Plasma - Mass Spectrometry (SF-ICP-MS). Among workers, 84% were exposed to DU, 9% to EU and DU, and 6% to natural uranium (NU) only. For those exposed to DU, urinary isotopic and [U] compositions result from binary mixing of NU and the DU plant feedstock. Among residents, 8% show evidence of DU exposure, whereas none shows evidence of EU exposure. For residents, the [U] geometric mean is significantly below the value reported for NHANES. There is no significant difference in [U] between exposed and unexposed residents, suggesting that [U] alone is not a reliable indicator of exposure to DU in this group. Ninety four percent of workers tested showed evidence of exposure to DU, EU or both, and were still excreting DU and EU decades after leaving the workforce. The study demonstrates the advantage of measuring multiple isotopic ratios (e.g., (236)U/(238)U and (235)U/(238)U) over a single ratio ((235)U/(238)U) in determining sources of uranium exposure. Copyright © 2016 Elsevier Inc. All rights reserved.

Late summer carbon export and remineralisation in the Southern Ocean determined with the combined 234Th and particulate biogenic Ba tracers

NASA Astrophysics Data System (ADS)

Planchon, F.; Cavagna, A.-J.; Cardinal, D.; André, L.; Dehairs, F.

2012-04-01

As part of the Bonus-GoodHope expedition (late summer 2008; Feb-March) in the Atlantic sector of the Southern Ocean, we present combined 234Th and biogenic particulate barium (Baxs) results. These data are used to estimate the export of particulate organic carbon (POC) from the upper mixed layer and the impact of twilight zone remineralisation on the carbon export. Total 234Th activity in surface waters is depleted relative to its parent nuclide 238U (234Th/238U ratio ranging from 0.74 to 0.91), while equilibrium is reached at the base of the surface mixed-layer. The export fluxes of 234Th from the 100m horizon, as estimated using steady state (SS) and non steady state (NSS) models, reveal different latitudinal trends. SS 234Th export varies from 496 dpm m-2 d-1 in the subtropical domain of the Cape Basin to 1195 dpm m-2 d-1 close to the Polar Front (PF). NSS export representative for a 15 to 22 day period preceding the cruise, is consistently less than SS export in the sub-Antarctic Zone (SAZ, 150 dpm m-2 d-1) and the Polar Frontal Zone (PFZ, 440 dpm m-2 d-1) but is similar further south in the Antarctic Zone (AZ, 1217 dpm m-2 d-1) and the northern Weddell Gyre (N-WG; 757 dpm m-2 d-1). This reflects temporal variability of export north of the PF, while south of the PF the export system appears to be in steady state during this late summer situation. The POC:Th ratio of large (>53 µm) particles collected below the surface mixed layer increases from 1.7 µmol dpm-1 in the STZ to a maximum of 4.8 µmol dpm-1 at the Southern Antarctic Circumpolar Current Front (SACCF), suggesting a southward increase of the contribution of larger cells, such as diatoms, to sinking material. Using these POC:Th ratios we calculate that the POC SS export from the 100m horizon reaches 0.9-1.7 mmol m-2 d-1 in the STZ and the SAZ, 2.6-4.7 mmol m-2 d-1 in the PFZ, and 3.3 mmol m-2 d-1 in the N-WG. Below the export layer, in the mesopelagic zone (100-600 m), 234Th activities generally reach equilibrium with 238U, but sometimes also are in large excess (234Th/238U ratio > to 1.1). Such activity excesses reflect intense remineralisation/disaggregation of 234Th-bearing particles which is estimated to attenuate the original POC export flux by close to 100%. Increased biogenic particulate Ba (Baxs) contents in the mesopelagic zone, indicate enhanced remaineralisation of organic matter, and in general overlap with the areas of excess 234Th. Excluding two outliers, we found a general positive correlation for mesopelagic waters between POC remineralisation estimated from Baxs inventories and from 234Th excess. Our results indicate that POC export production in the Southern Ocean is strongly attenuated in the mesopelagic waters.

Calibrating multiple isotopic proxies in a modern aragonite speleothem from northeast India

NASA Astrophysics Data System (ADS)

Ronay, E.; Oster, J. L.; Sharp, W. D.; Marks, N.; Erhardt, A.; Breitenbach, S. F. M.

2017-12-01

Uranium, strontium, and calcium isotope ratios in calcite speleothems are used as proxies for water-soil-rock interactions and prior calcite precipitation, and thus provide information about effective rainfall amount variations, primarily in semi-arid or highly seasonal regions. However, less is known about how these proxies function in humid regions and in aragonite speleothems. In this study, we use meteorological data to calibrate (234U/238U)i and 87Sr/86Sr in a modern aragonite speleothem from northeast India, the rainiest place on Earth, to determine how these proxies reflect effective monsoon rainfall amount. MAW-0201 is an annually laminated aragonite stalagmite that grew from 1960-2013 in Mawmluh Cave, Meghalaya, India. Rainfall here is extremely seasonal due to the Indian Summer Monsoon (ISM), which brings several meters of rain to the region each summer, but with inter-annual variability in total rainfall. The δ18O in Mawmluh dripwater and speleothems reflects moisture source and transport, rather than rainfall amount. Variations in Mg, U, and Ba concentrations in MAW-0201 show seasonal and multi-annual variability. U and Mg are closely correlated, but multi-year periods show significant anti-correlation. The Mg and U distribution coefficients in calcite and aragonite indicate correlated periods are times of prior calcite precipitation (PCP) and anti-correlated periods are times of prior aragonite precipitation (PAP) in the epikarst. We use δ44/40Ca to test this hypothesis, as Ca isotopes fractionate differently during calcite and aragonite precipitation and speleothem δ44/40Ca will record unique PAP and PCP fingerprints. We propose such shifts from PCP to PAP reflect hydrologic variability and/or flow path changes, which provide a useful tool for understanding epikarst hydrology but may also be a complicating factor in speleothem-based paleoclimate interpretations. Preliminary (234U/238U)i (always <1) and 87Sr/86Sr spanning 1991-2009 each show significant variability outside of analytical error. (234U/238U)i displays a decadal trend, gradually increasing until 2000 and decreasing to the end of the record. Several years in the 87Sr/86Sr record have anomalously high values, which may reflect increased sea spray input and provide unique information on the wind component of the ISM.

Potential human health risk by metal(loid)s, 234,238U and 210Po due to consumption of fish from the "Luis L. Leon" Reservoir (Northern México).

PubMed

Luna-Porres, Mayra Y; Rodríguez-Villa, Marco A; Herrera-Peraza, Eduardo F; Renteria-Villalobos, Marusia; Montero-Cabrera, María E

2014-06-25

Concentrations of As, Cu, Fe, Hg, Pb and Zn and activity concentrations from 234,238U and 210Po in water, fillet, liver and gills were determined in three stocked fish species from the Luis L. Leon reservoir, located in Northern Mexico. The considered species were Lepomis cyanellus, Cyprinus carpio and Ictalurus furcatus. 238U and 234U activity concentration (AC) in fillet samples showed values of 0.007-0.014 and 0.01-0.02 Bq∙kg-1 wet weight (ww), respectively. Liver samples for L. cyanellus, C. carpio and I. furcatus present 210Po AC of 1.16-3.26, 0.70-1.13 and 0.93-1.37 Bq∙kg-1 ww. Arsenic, mercury and lead concentration intervals in fillet samples were 0.13-0.39, 0.005-0.126 and 0.009-0.08 mg∙kg-1 ww, respectively, while in gill samples they were 0.11-0.43, 0.002-0.039 and 0.02-0.26 mg∙kg-1 ww. The elemental Bioaccumulation Factor (BAF) for fish tissues with respect to their concentrations in water was determined. L. cyanellus showed the highest BAF values for As and total U, being BAFAs = 37 and 40 L∙kg-1 in fillet and gills, respectively, and BAFU total = 1.5 L∙kg-1 in fillet. I. furcatus showed the highest BAF values for Hg and Pb, being BAFHg = 40 and 13 L∙kg-1 in fillet and gills, and BAFPb = 6.5 and 22 L∙kg-1 in fillet and gills, respectively. Some metal(loid) concentrations are slightly higher than European regulations for fish fillets. The difference in concentrations of metal(loid)s in fillet among the studied species is probably due to their differences in diet and habitat.

Potential Human Health Risk by Metal(loid)s, 234,238U and 210Po due to Consumption of Fish from the “Luis L. Leon” Reservoir (Northern México)

PubMed Central

Luna-Porres, Mayra Y.; Rodríguez-Villa, Marco A.; Herrera-Peraza, Eduardo F.; Renteria-Villalobos, Marusia; Montero-Cabrera, María E.

2014-01-01

Concentrations of As, Cu, Fe, Hg, Pb and Zn and activity concentrations from 234,238U and 210Po in water, fillet, liver and gills were determined in three stocked fish species from the Luis L. Leon reservoir, located in Northern Mexico. The considered species were Lepomis cyanellus, Cyprinus carpio and Ictalurus furcatus. 238U and 234U activity concentration (AC) in fillet samples showed values of 0.007–0.014 and 0.01–0.02 Bq∙kg−1 wet weight (ww), respectively. Liver samples for L. cyanellus, C. carpio and I. furcatus present 210Po AC of 1.16–3.26, 0.70–1.13 and 0.93–1.37 Bq∙kg−1 ww. Arsenic, mercury and lead concentration intervals in fillet samples were 0.13–0.39, 0.005–0.126 and 0.009–0.08 mg∙kg−1 ww, respectively, while in gill samples they were 0.11–0.43, 0.002–0.039 and 0.02–0.26 mg∙kg−1 ww. The elemental Bioaccumulation Factor (BAF) for fish tissues with respect to their concentrations in water was determined. L. cyanellus showed the highest BAF values for As and total U, being BAFAs = 37 and 40 L∙kg−1 in fillet and gills, respectively, and BAFU total = 1.5 L∙kg−1 in fillet. I. furcatus showed the highest BAF values for Hg and Pb, being BAFHg = 40 and 13 L∙kg−1 in fillet and gills, and BAFPb = 6.5 and 22 L∙kg−1 in fillet and gills, respectively. Some metal(loid) concentrations are slightly higher than European regulations for fish fillets. The difference in concentrations of metal(loid)s in fillet among the studied species is probably due to their differences in diet and habitat. PMID:24968208

Sequential Determination of U and Th Decay Series in Santana Cave, Southwest Brazil

NASA Astrophysics Data System (ADS)

Silva, P. S. C.; Damatto, S. R.; Mazzilli, B. P.

2008-08-01

Parque Estadual Turístico do Alto Ribeira (PETAR) is located in the South-western part of São Paulo State, in the Ribeira Valley. In this national state park a large number of caves are found, which are among the most visited of the country. These caves, located in a karstic zone, are characterized by the presence of carbonaceous rocks frequently fractured and collapsed. Although, carbonates (dolomites and calcitic rocks) usually have low U content, this element can be found in the structure of the surrounding rocks. This paper aims to determine 238U, 234U, 226Ra and 210Pb concentration in samples of rock, soil, river water and sediment, in Santana cave. The radionuclide 238U was determined by alpha spectrometry using a surface barrier detector. 226Ra and 210Pb were determined by measuring the gross alpha and beta activity on a gas flow proportional counter.

Temporal Variations in 234U/238U Activity Ratios in the Lower Mississippi River due to Changes in Source Tributary Discharges

NASA Astrophysics Data System (ADS)

Grzymko, T. J.; Marcantonio, F.; McKee, B. A.; Stewart, C. M.

2004-12-01

The world's 25 largest river systems contribute nearly 50% of all freshwater to the global ocean and carry large quantities of dissolved trace metals annually. Trace metal concentrations in these systems show large variances on seasonal time scales. In order to constrain the causes of these variations, consistent sampling on sub-seasonal time intervals is essential. Here, we focus on the Mississippi River, the seventh largest river in the world in terms of freshwater discharge and the third largest in terms of drainage basin area. Biweekly sampling of the lower Mississippi River at New Orleans was performed from January 2003 to August 2004. Uranium concentrations and 234U/238U activity ratios were measured for the dissolved component (<0.2 μ m-fraction) of river water. Over the course of this study, dissolved U activity ratios spanned a range of about 25%, from 1.23 to 1.60. Dissolved U concentrations ranged from 0.28 to 1.06 ppb. The relationship between concentrations, activity ratios, and lower river discharge is complicated, and no clear pattern is observed on both biweekly and seasonal timescales. However, there does seem to be a relationship between the larger seasonal trends in the lower Mississippi River and variations in the discharge of its upstream tributaries. To constrain this relationship, we have sampled water from the Missouri River, the upper Mississippi River above the confluence with the Missouri, the Ohio River, and the Arkansas River in February, April, and August of 2004. For the upstream samples measured thus far, the highest dissolved uranium concentrations are observed for the Missouri River at 2.02 ppb, while the lowest are found in the Ohio River at 0.38 ppb. Dissolved 234U/238U activity ratios are as unique for each tributary and vary from 1.36 in the Ohio River to 1.51 in the Missouri River. A preliminary mass balance analysis reveals that the lower river uranium activity ratios are controlled simply by the quantity and isotope signature of the waters discharged from the upstream tributaries. A discussion of the implications of this work for global ocean budgets of uranium will be presented.

Influence of a Decaying Cyclonic Eddy on Biogenic Silica and Particulate Organic Carbon in the Tropical South China Sea Based on 234Th-238U Disequilibrium.

PubMed

Yang, Weifeng; Chen, Min; Zheng, Minfang; He, Zhigang; Zhang, Xinxing; Qiu, Yusheng; Xu, Wangbin; Ma, Lili; Lin, Zhiyu; Hu, Wangjiang; Zeng, Jian

2015-01-01

Eddies play a critical role in regulating the biological pump by pumping new nutrients to the euphotic zone. However, the effects of cyclonic eddies on particle export are not well understood. Here, biogenic silica (BSi) and particulate organic carbon (POC) exports were examined inside and outside a decaying cyclonic eddy using 234Th-238U disequilibria in the tropical South China Sea. For the eddy and outside stations, the average concentrations of BSi in the euphotic zone were 0.17±0.09 μmol L-1 (mean±sd, n = 20) and 0.21±0.06 μmol L-1 (n = 34). The POC concentrations were 1.42±0.56 μmol L-1 (n = 34) and 1.30±0.46 μmol L-1 (n = 51). Both BSi and POC abundances did not show change at the 95% confidence level. Based on the 234Th-238U model, BSi export fluxes in the eddy averaged 0.18±0.15 mmol Si m-2 d-1, which was comparable with the 0.40±0.20 mmol Si m-2 d-1 outside the eddy. Similarly, the average POC export fluxes were 1.5±1.4 mmol C m-2 d-1 and 1.9±1.3 mmol C m-2 d-1 for the eddy and outside stations. From these results we concluded that cyclonic eddies in their decaying phase have little effect on the abundance and export of biogenic particles.

Influence of a Decaying Cyclonic Eddy on Biogenic Silica and Particulate Organic Carbon in the Tropical South China Sea Based on 234Th-238U Disequilibrium

PubMed Central

Yang, Weifeng; Chen, Min; Zheng, Minfang; He, Zhigang; Zhang, Xinxing; Qiu, Yusheng; Xu, Wangbin; Ma, Lili; Lin, Zhiyu; Hu, Wangjiang; Zeng, Jian

2015-01-01

Eddies play a critical role in regulating the biological pump by pumping new nutrients to the euphotic zone. However, the effects of cyclonic eddies on particle export are not well understood. Here, biogenic silica (BSi) and particulate organic carbon (POC) exports were examined inside and outside a decaying cyclonic eddy using 234Th-238U disequilibria in the tropical South China Sea. For the eddy and outside stations, the average concentrations of BSi in the euphotic zone were 0.17±0.09 μmol L-1 (mean±sd, n = 20) and 0.21±0.06 μmol L-1 (n = 34). The POC concentrations were 1.42±0.56 μmol L-1 (n = 34) and 1.30±0.46 μmol L-1 (n = 51). Both BSi and POC abundances did not show change at the 95% confidence level. Based on the 234Th-238U model, BSi export fluxes in the eddy averaged 0.18±0.15 mmol Si m-2 d-1, which was comparable with the 0.40±0.20 mmol Si m-2 d-1 outside the eddy. Similarly, the average POC export fluxes were 1.5±1.4 mmol C m-2 d-1 and 1.9±1.3 mmol C m-2 d-1 for the eddy and outside stations. From these results we concluded that cyclonic eddies in their decaying phase have little effect on the abundance and export of biogenic particles. PMID:26317555

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+-bearing) structures will tend to have higher 238U/235U than uranate-type structures that lack strong U=O bonds. References: 1. Bigeleisen (1996) JACS 118:3676; 2. Schauble (2006) Eos 87:V21B-0570; 3. Abe et al. (2008) J Chem Phys 128:144309, 129:164309, & Abe et al. (2010) J Chem Phys 133:044309; 4. Schauble (2013) PNAS 110:17714.

Selective recovery of uranium from Ca-Mg uranates by chlorination

NASA Astrophysics Data System (ADS)

Pomiro, Federico J.; Gaviría, Juan P.; Quinteros, Raúl D.; Bohé, Ana E.

2017-07-01

A chlorination process is proposed for the uranium extraction and separation using Calciumsbnd Magnesium uranates such as starting reactants which were obtained by precipitation from uranyl nitrate solutions with calcium hydroxide. The study is based on thermodynamic and reaction analysis using chlorine gas as chlorination agent. The results showed that the chlorination reaction of Ca uranate is more feasible to occur than the Mg uranate. The products obtained after chlorination reactions were washed with deionized water to remove the chlorides produced and analyzed. The XRD patterns of the washed products indicated that the chlorination between 400 and 500 °C result in a single phase of calcium uranate (CaUO4) as reaction product. The formation of U3O8 and MgU3O10 was observed at temperatures between 600 °C and 700 °C for 8 hs. The optimal conditions to recover uranium were 3 l h-1 of chlorine and 10 hs of reaction at 700 °C being U3O8 the single uranium product obtained.

Plutonium age dating reloaded

NASA Astrophysics Data System (ADS)

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

2014-05-01

Although the age determination of plutonium is and has been a pillar of nuclear forensic investigations for many years, additional research in the field of plutonium age dating is still needed and leads to new insights as the present work shows: Plutonium is commonly dated with the help of the 241Pu/241Am chronometer using gamma spectrometry; in fewer cases the 240Pu/236U chronometer has been used. The age dating results of the 239Pu/235U chronometer and the 238Pu/234U chronometer are scarcely applied in addition to the 240Pu/236U chronometer, although their results can be obtained simultaneously from the same mass spectrometric experiments as the age dating result of latter. The reliability of the result can be tested when the results of different chronometers are compared. The 242Pu/238U chronometer is normally not evaluated at all due to its sensitivity to contamination with natural uranium. This apparent 'weakness' that renders the age dating results of the 242Pu/238U chronometer almost useless for nuclear forensic investigations, however turns out to be an advantage looked at from another perspective: the 242Pu/238U chronometer can be utilized as an indicator for uranium contamination of plutonium samples and even help to identify the nature of this contamination. To illustrate this the age dating results of all four Pu/U clocks mentioned above are discussed for one plutonium sample (NBS 946) that shows no signs of uranium contamination and for three additional plutonium samples. In case the 242Pu/238U chronometer results in an older 'age' than the other Pu/U chronometers, contamination with either a small amount of enriched or with natural or depleted uranium is for example possible. If the age dating result of the 239Pu/235U chronometer is also influenced the nature of the contamination can be identified; enriched uranium is in this latter case a likely cause for the missmatch of the age dating results of the Pu/U chronometers.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cherdyntsev, V.V.; Kazachevskii, I.V.; Kuzmina, E.A.

The ratio of Th isotopes (Io,/sup -/UX/sub 1/, Th/sup 232/, RdTh) and U isotopes (U/sup 234/ and U/sup 238/) in natural waters, fossil bones, and soils, as well as in shells of fresh-water mollusks of the Paleolithic site Molodovo and other areas of the Dniester foreland was investigated. In the waters of Molodovo are distinguished waters of neogenic limestones with a low value of gamma =U/sup 234//U/sup 238/ = 10.3 x 10.5 and waters of the Paleozoic: gamma = 1.34, apparently feeding the quarternary stratum. The mineralization of fossil bones was realized in the Upper Paleolith by waters with lowmore » values and in the Middle Paleolith by waters with high gamma -values. Uranium migration was confirmed by the investigation of the radioelement ratios in fossil bones of the sites Molodovo I and Molodovo V. This process apparently did not affect the Mousterian layers of the site Molodovo V, so that the age of the layers, according to Io/UX/sub 1/ and gamma , equaling 130 thousand years, is near to the truth. The age of the fossil soil of the lower horizon of Molodovo I (end of Riss -RissWurm) is more than 260 thousand years. In the shells of fresh-water mollusks an intensive migration of U and Ra isotopes occurs For example, an exceptional high value RdTh/Th = 12.3 450 deg C in a 0.9 (activity units) was obtained. (auth)« less

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.

U–Pb, Rb–Sr, and U-series isotope geochemistry of rocks and fracture minerals from the Chalk River Laboratories site, Grenville Province, Ontario, Canada

USGS Publications Warehouse

Neymark, Leonid; Peterman, Zell E.; Moscati, Richard J.; Thivierge, R. H.

2013-01-01

As part of the Geologic Waste Management Facility feasibility study, Atomic Energy of Canada Ltd. (AECL) is evaluating the suitability of the Chalk River Laboratories (CRL) site in Ontario, situated in crystalline rock of the southwestern Grenville Province, for the possible development of an underground repository for low- and intermediate-level nuclear waste. This paper presents petrographic and trace element analyses, U–Pb zircon dating results, and Rb–Sr, U–Pb and U-series isotopic analyses of gneissic drill core samples from the deep CRG-series characterization boreholes at the CRL site. The main rock types intersected in the boreholes include hornblende–biotite (±pyroxene) gneisses of granitic to granodioritic composition, leucocratic granitic gneisses with sparse mafic minerals, and garnet-bearing gneisses with variable amounts of biotite and/or hornblende. The trace element data for whole-rock samples plot in the fields of within-plate, syn-collision, and volcanic arc-type granites in discrimination diagrams used for the tectonic interpretation of granitic rocks.Zircons separated from biotite gneiss and metagranite samples yielded SHRIMP-RG U–Pb ages of 1472 ± 14 (2σ) and 1045 ± 6 Ma, respectively, in very good agreement with widespread Early Mesoproterozoic plutonic ages and Ottawan orogeny ages in the Central Gneiss Belt. The Rb–Sr, U–Pb, and Pb–Pb whole-rock errorchron apparent ages of most of the CRL gneiss samples are consistent with zircon U–Pb age and do not indicate substantial large-scale preferential element mobility during superimposed metamorphic and water/rock interaction processes. This may confirm the integrity of the rock mass, which is a positive attribute for a potential nuclear waste repository. Most 234U/238U activity ratios (AR) in whole rock samples are within errors of the secular equilibrium value of one, indicating that the rocks have not experienced any appreciable U loss or gain within the past 1 Ma. However, 234U/238U AR in fracture mineral samples collected down to borehole lengths of about 740 m deviate from the secular equilibrium value and 234U/238U model ages calculated for fracture mineral samples showing excess 234U range from 593 to 1415 ka, thus providing evidence of fracture flow in the associated bedrock during the past 1.5 Ma. Rare earth element patterns are variable in fracture-filling calcites and Fe oxides/hydroxides but are similar to those observed in associated whole-rock samples. The observed Ce anomalies are very small (CeN/CeN∗≈1">CeN/CeN∗≈1), do not vary with depth, and, therefore, do not contain evidence that the studied fracture minerals precipitated from oxidizing waters at the conceptual depth of a repository.

Natural radioactivity in underground water from the Outer Carpathians in Poland with the use of nuclear spectrometry techniques.

PubMed

Walencik, A; Kozłowska, B; Dorda, J; Zipper, W

2010-01-01

The investigations of natural radioactivity in underground mineral water and spring water in health resorts in the Outer Carpathians were performed. Samples from 40 water springs were collected 3-4 times over a period of 10 years (1997-2007). In order to obtain necessary data, two different nuclear spectrometry techniques were applied: WinSpectral alphabeta 1414 liquid scintillation counter from Wallac and alpha-spectrometer 7401 VR from Canberra-Packard, USA with the silicon surface barrier detector. The activity concentrations of (222)Rn in the investigated samples varied from below 1 to 50 Bq/l. For radium isotopes the concentrations were in a range from below 10 to 490 mBq/l for (226)Ra and from 29 to 397 mBq/l for (228)Ra. The highest concentrations for both radium isotopes were obtained for medicinal water Zuber III from Krynica spa. The activity concentrations for uranium isotopes varied from below 0.5 to 16 mBq/l for (238)U and from below 0.5 to 162 mBq/l for (234)U with the highest values obtained for water Zuber IV. The highest annual effective dose arising from mainly radium isotopes was obtained for Zuber III water and was equal to 75 microSv/yr. Additionally, the annual effective doses due to (222)Rn consumed with water were also estimated. The isotopic ratios between isotopes originating from the same decay chain ((234)U/(238)U, (226)Ra/(238)U) and from different radioactive decay chains ((226)Ra/(228)Ra) were determined. The correlations between different isotopes were presented. Copyright 2009 Elsevier Ltd. All rights reserved.

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

PubMed

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

2016-03-01

The preparation and characterization of certified reference materials (CRMs) for radionuclide content in sediments collected offshore of Bikini Atoll (IAEA-410) and in the open northwest Pacific Ocean (IAEA-412) are described and the results of the certification process are presented. The certified radionuclides include: (40)K, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (234)U, (238)U, (239)Pu, (239+240)Pu and (241)Am for IAEA-410 and (40)K, (137)Cs, (210)Pb ((210)Po), (226)Ra, (228)Ra, (228)Th, (232)Th, (235)U, (238)U, (239)Pu, (240)Pu and (239+240)Pu for IAEA-412. The CRMs can be used for quality assurance and quality control purposes in the analysis of radionuclides in sediments, for development and validation of analytical methods and for staff training. Copyright © 2015 Elsevier Ltd. All rights reserved.

Constraining the calculation of 234,236,238U (n ,γ ) cross sections with measurements of the γ -ray spectra at the DANCE facility

NASA Astrophysics Data System (ADS)

Ullmann, J. L.; Kawano, T.; Baramsai, B.; Bredeweg, T. A.; Couture, A.; Haight, R. C.; Jandel, M.; O'Donnell, J. M.; Rundberg, R. S.; Vieira, D. J.; Wilhelmy, J. B.; Krtička, M.; Becker, J. A.; Chyzh, A.; Wu, C. Y.; Mitchell, G. E.

2017-08-01

The cross section for neutron capture in the continuum region has been difficult to calculate accurately. Previous results for 238U show that including an M 1 scissors-mode contribution to the photon strength function resulted in very good agreement between calculation and measurement. This paper extends that analysis to U,236234 by using γ -ray spectra measured with the Detector for Advanced Neutron Capture Experiments (DANCE) at the Los Alamos Neutron Science Center to constrain the photon strength function used to calculate the capture cross section. Calculations using a strong scissors-mode contribution reproduced the measured γ -ray spectra and were in excellent agreement with the reported cross sections for all three isotopes.

Fission cross sections of some thorium, uranium, neptunium and plutonium isotopes relative to /sup 235/U

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meadows, J W

1983-10-01

Earlier results from the measurements, at this Laboratory, of the fission cross sections of /sup 230/Th, /sup 232/Th, /sup 233/U, /sup 234/U, /sup 236/U, /sup 238/U, /sup 237/Np, /sup 239/Pu, /sup 240/Pu, and /sup 242/Pu relative to /sup 235/U are reviewed with revisions to include changes in data processing procedures, alpha half lives and thermal fission cross sections. Some new data have also been included. The current experimental methods and procedures and the sample assay methods are described in detail and the sources of error are presented in a systematic manner. 38 references.

Sequential Determination of U and Th Decay Series in Santana Cave, Southwest Brazil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Silva, P. S. C.; Damatto, S. R.; Mazzilli, B. P.

2008-08-07

Parque Estadual Turistico do Alto Ribeira (PETAR) is located in the South-western part of Sao Paulo State, in the Ribeira Valley. In this national state park a large number of caves are found, which are among the most visited of the country. These caves, located in a karstic zone, are characterized by the presence of carbonaceous rocks frequently fractured and collapsed. Although, carbonates (dolomites and calcitic rocks) usually have low U content, this element can be found in the structure of the surrounding rocks. This paper aims to determine {sup 238}U, {sup 234}U, {sup 226}Ra and {sup 210}Pb concentration inmore » samples of rock, soil, river water and sediment, in Santana cave. The radionuclide {sup 238}U was determined by alpha spectrometry using a surface barrier detector. {sup 226}Ra and {sup 210}Pb were determined by measuring the gross alpha and beta activity on a gas flow proportional counter.« less

Applications of New Synthetic Uranium Reference Materials for Geochemistry Research (Invited)

NASA Astrophysics Data System (ADS)

Richter, S.; Weyer, S.; Alonso, A.; Aregbe, Y.; Kuehn, H.; Eykens, R.; Verbruggen, A.; Wellum, R.

2009-12-01

For many applications in geochemistry research isotope ratio measurements play a significant role. In geochronology isotope abundances of uranium and its daughter products thorium and lead are being used to determine the age and history of various samples of geological interest. For measuring the isotopic compositions of these elements by mass spectrometry, suitable isotope reference materials are needed to validate measurement procedures and to calibrate multi-collector and ion counting detector systems. IRMM is a recognized provider for nuclear isotope reference materials to the nuclear industry and nuclear safeguards authorities, which are also being applied widely for geochemical applications. The preparation of several new synthetic uranium reference materials at IRMM during the recent five years has provided significant impacts on geochemical research. As an example, the IRMM-074 series of gravimetrically prepared uranium mixtures for linearity testing of secondary electron multipliers (SEMs) has been applied for the redetermination of the secular equilibrium 234U/238U value and the 234U half-life by Cheng et al (2009). Due to the use of IRMM-074, results with smaller uncertainties were obtained, which are shifted by about 0.04% compared to the commonly used values published earlier by Cheng et al. in 2000. This has a significant impact for U isotope measurements in geochemistry.. As a further example, the new double spike IRMM-3636 with a 233U/236U ratio of 1:1 and an expanded uncertainty as low as 0.016% (coverage factor k=2, 95% confidence level) was prepared gravimetrically. This double spike allows internal mass fractionation correction for high precision 235U/238U ratio measurements of close to natural samples. Using the new double spike IRMM-3636, the 235U/238U ratios for several commonly used natural U standard materials from NIST/NBL and IRMM, such as e.g. NBS960 (=NBL CRM-112a), NBS950a,b and IRMM-184, have been re-measured with improved precision and accuracy. The (preliminary) result of 137.836(23) for the 238U/235U ratio of NBS960, measured using the new gravimetrically prepared 233U/236U-Double Spike IRMM-3636, is deviating by -0.032% from the well-known and widely used consensus value of 137.88. For the consensus value no uncertainty has ever been assigned, but it is outside the uncertainty limits of the new measurement result. The re-measured 238U/235U ratio of 137.689(22) of IRMM-184 agrees quite well with the certified value of 137.697(41), the calculated difference is only -0.006(34)% which is insignificant. The results for both NBS960 and IRMM-184, obtained using multi-dynamic TIMS at IRMM and using high efficiency MC-ICPMS at the University of Frankfurt, agree well with each other. As a conclusion, the IRMM-3636 Double Spike has been successfully applied for measurements of important uranium isotopic standards like NBS960 and IRMM-184, with improved uncertainties at the level of 0.016%.

Effects of surface-water irrigation on sources, fluxes, and residence times of water, nitrate, and uranium in an alluvial aquifer

USGS Publications Warehouse

Böhlke, J.K.; Verstraeten, Ingrid M.; Kraemer, T.F.

2007-01-01

Effects of surface-water irrigation on an alluvial aquifer were evaluated using chemical and isotopic data including ??2H, ??18O, 3H, ??3He, Ar, Ne, N2, ??15N, and 234U/238U activity ratios in a transect of nested wells in the North Platte River valley in western Nebraska, USA. The data were used to evaluate sources and fluxes of H2O, NO3- and U, all of which were strongly affected by irrigated agriculture. Combined results indicate that the alluvial aquifer was dominated by irrigation water that had distinctive chemical and isotopic features that were inherited from the North Platte River or acquired from agricultural soils or recharge processes. Values of ??2H, ??18O, Ar and Ne indicate that most of the ground water in the alluvial aquifer was irrigation water that was derived from the North Platte River and distributed during the growing season. The irrigation water was identified by an evaporated isotopic signature that was acquired by the river in major upstream reservoirs in Wyoming, and by relatively warm gas-equilibration temperatures related to warm-season recharge. Apparent 3H-3He ages indicate that the ground water in the alluvium was stratified and mostly 3.0 m/a. Age gradients and NO3- concentrations indicate that recharge occurred by a combination of focused leakage from irrigation canals (rapid local recharge, low NO3-) and distributed infiltration beneath the irrigated agricultural fields (lower recharge, high NO3-). Large amounts of U with relatively low 234U/238U activity ratios were present in the alluvial aquifer as a result of irrigation with U-bearing river water, and minor amounts of U with higher 234U/238U activity ratios were added locally from basal and underlying volcanic-rich sediments. Distributions of NO3-, ?? 15 N [NO3-], dissolved gases, and ground-water ages indicate that NO3- concentrations increased and ?? 15 N [NO3-] values decreased in distributed recharge in the last few decades, possibly in relation to a documented increase in the agricultural use of artificial fertilizers. Canal leakage caused substantial dilution of NO3- within the alluvial aquifer, whereas denitrification occurred mainly near the bottom of the alluvium. The average residence time of the irrigation water within the aquifer was relatively short (about 9 a) and reactions such as respiration, denitrification and U exchange in the saturated zone had relatively little effect on the overall composition of the alluvial ground water in comparison to what they might have had in the absence of irrigation recharge.

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

PubMed

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

2014-04-01

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

Actinides in deer tissues at the rocky flats environmental technology site.

PubMed

Todd, Andrew S; Sattelberg, R Mark

2005-11-01

Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range.

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.

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.

Direct comparison of 210Po, 234Th and POC particle-size distributions and export fluxes at the Bermuda Atlantic Time-series Study (BATS) site.

PubMed

Stewart, Gillian; Moran, S Bradley; Lomas, Michael W; Kelly, Roger P

2011-05-01

Particle-reactive, naturally occurring radionuclides are useful tracers of the sinking flux of organic matter from the surface to the deep ocean. Since the Joint Global Ocean Flux Study (JGOFS) began in 1987, the disequilibrium between (234)Th and its parent (238)U has become widely used as a technique to measure particle export fluxes from surface ocean waters. Another radionuclide pair, (210)Po and (210)Pb, can be used for the same purpose but has not been as widely adopted due to difficulty with accurately constraining the (210)Po/(210)Pb radiochemical balance in the ocean and because of the more time-consuming radiochemical procedures. Direct comparison of particle flux estimated in different ocean regions using these short-lived radionuclides is important in evaluating their utility and accuracy as tracers of particle flux. In this paper, we present paired (234)Th/(238)U and (210)Po/(210)Pb data from oligotrophic surface waters of the subtropical Northwest Atlantic and discuss their advantages and limitations. Vertical profiles of total and particle size-fractionated (210)Po and (234)Th activities, together with particulate organic carbon (POC) concentrations, were measured during three seasons at the Bermuda Atlantic Time-series Study (BATS) site. Both (210)Po and (234)Th reasonably predict sinking POC flux caught in sediment traps, and each tracer provides unique information about the magnitude and efficiency of the ocean's biological pump. Copyright © 2010 Elsevier Ltd. All rights reserved.

Uranium isotopes (U-234/U-238) in rivers of the Yukon Basin (Alaska and Canada) as an aid in identifying water sources, with implications for monitoring hydrologic change in arctic regions

USGS Publications Warehouse

Kraemer, Thomas F.; Brabets, Timothy P.

2012-01-01

The ability to detect hydrologic variation in large arctic river systems is of major importance in understanding and predicting effects of climate change in high-latitude environments. Monitoring uranium isotopes (234U and 238U) in river water of the Yukon River Basin of Alaska and northwestern Canada (2001–2005) has enhanced the ability to identify water sources to rivers, as well as detect flow changes that have occurred over the 5-year study. Uranium isotopic data for the Yukon River and major tributaries (the Porcupine and Tanana rivers) identify several sources that contribute to river flow, including: deep groundwater, seasonally frozen river-valley alluvium groundwater, and high-elevation glacial melt water. The main-stem Yukon River exhibits patterns of uranium isotopic variation at several locations that reflect input from ice melt and shallow groundwater in the spring, as well as a multi-year pattern of increased variability in timing and relative amount of water supplied from higher elevations within the basin. Results of this study demonstrate both the utility of uranium isotopes in revealing sources of water in large river systems and of incorporating uranium isotope analysis in long-term monitoring of arctic river systems that attempt to assess the effects of climate change.

U, Th and Pa insights into sedimentological and paleoceanographic changes off Hudson Strait (Labrador Sea) during the last ∼37 ka with special attention to methodological issues

NASA Astrophysics Data System (ADS)

Nuttin, Laurence; Maccali, Jenny; Hillaire-Marcel, Claude

2015-05-01

A ∼9 m-long sediment core spanning the last ∼37 ka has been raised from the lower Labrador continental slope, off the Hudson Strait shelf edge. It has been analyzed for its U, Th and Pa isotope contents, along with current sedimentological parameters, as a means to retrieve information about sedimentological changes in response to northeastern Laurentide Ice Sheet (LIS) margin instabilities. The sequence yielded a high-resolution record of subglacial detrital carbonate pulses from Hudson Strait assigned to "Heinrich events" H2 and H1, whereas H0 was missing. Large variations in bulk sediment U- and Th-contents as well as in 234U/238U activity ratio are observed throughout the sequence, leading to large uncertainties when calculating excesses in 231Pa and 230Th (231Paxs and 230Thxs) over their supported and in-growth fractions (i.e., inherited from detrital minerals and produced from authigenic and diagenetic U-uptake). In particular, 234U excesses or deficits vs 238U (-115‰ < δ234U < +126‰) are observed throughout the sequence, suggesting occasional U-uptake from the water column and/or some late diagenetic mobility along discrete redox gradients, despite the overall low and little variable organic carbon content (0.3 ± 0.1%) observed. The above uncertainties in 231Paxs and 230Thxs estimates and the large variability in geochemical and sedimentary fluxes off the northeastern LIS margin, lead us to downgrade the potential paleoceanographic information yielded by these isotopes in such a setting. Nonetheless, the H2 and H1 layers are highlighted by very low initial excesses in both 230Thxs and 231Paxs, indicating their extremely fast deposition. Throughout most of the sedimentary sequence, the calculated initial 230Thxs fluxes are nearly in balance with 230Th production in the overlying water column. Exceptions are the H2 layer, an interval succeeding H1, and the post-glacial sediment. The estimated initial (231Paxs/230Thxs) ratios are generally lower than their production rate in the water column (i.e., 0.092), indicating nearly continuous preferential export of 231Paxs over the last ∼37 cal ka BP, thus the persistence of some deep currents throughout the interval.

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 is required. We suggest a set of input parameter values for such a purpose. Additional considerations for calculating comminution ages of sediments deposited within large, semi-arid drainage basins are discussed.

A Record of Uranium-Series Transport in Fractured, Unsaturated Tuff at Nopal I, Sierra Peña Blanca, Chihuahua, Mexico

NASA Astrophysics Data System (ADS)

Denton, J.; Goldstein, S. J.; Paviet, P.; Nunn, A. J.; Amato, R. S.; Hinrichs, K. A.

2015-12-01

In this study we utilize U-series disequilibria measurements to investigate mineral fluid interactions and the role fractures play in the geochemical evolution of an analogue for a high level nuclear waste repository, the Nopal I uranium ore deposit. Samples of fracture-fill materials have been collected from a vertical drill core and surface fractures. High uranium concentrations in these materials (12-7700 ppm) indicate U mobility and transport from the deposit in the past. U concentrations generally decrease with horizontal distance away from the ore deposit but show no trend with depth. Isotopic activity ratios indicate a complicated geochemical evolution in terms of the timing and extent of actinide mobility, possibly due to changing environmental (redox) conditions over the history of the deposit. 234U/238U activity ratios are generally distinct from secular equilibrium and indicate some degree of open system U behavior during the past 1.2 Ma. However, calculated closed system 238U-234U-230Th model ages are generally >313 ka and >183 ka for the surface fracture and drill core samples respectively, suggesting closed system behavior for U and Th over this most recent time period. Whole rock isochrons drawn for the drill core samples show that at two of three depths fractures have remained closed with respect to U and Th mobility for >200 ka. However, open system behavior for U in the last 350 ka is suggested at 67 m depth. 231Pa/235U activity ratios within error of unity suggest closed system behavior for U and Pa for at least the past 185 ka. 226Ra/230Th activity ratios are typically <1 (0.7-1.2), suggesting recent (<8 ka) radium loss and mobility due to ongoing fluid flow in the fractures. Overall, the mainly closed system behavior of U-Th-Pa over the past ~200 ka provides one indicator of the geochemical immobility of these actinides over long time-scales for potential nuclear waste repositories sited in fractured, unsaturated tuff.

210Po and 238U isotope concentrations in commercial bottled mineral water samples in Spain and their dose contribution.

PubMed

Díaz-Francés, I; Mantero, J; Manjón, G; Díaz, J; García-Tenorio, R

2013-09-01

(210)Po is a naturally occurring radionuclide, belonging to the uranium series, which is present in minute amounts in the different environmental compartments (water, soil, biota). Through its route along the trophic chain, it can be incorporated in the human body via ingestion of waters and/or food. This radionuclide is highly radiotoxic, being one of the main contributors to the committed effective dose via ingestion by the general population. In this work, the contribution of this radionuclide to the committed effective dose received by the Spanish population via consumption of bottled mineral waters is evaluated. With this end, the (210)Po activity concentrations in a total of 32 different commercial bottled mineral waters have been determined by alpha-particle spectrometry. The determined contribution is also compared with the contributions of other natural radionuclides such as (234)U and (238)U.

Relatively Recent Volcanism on Oahu, Hawaii: New U-series and Paleomagnetic Age Constraints on the Hanauma Bay Eruption

NASA Astrophysics Data System (ADS)

Rubin, K. H.; Jurado-Chichay, Z.; Urrutia-Fucugauchi, J.

2002-12-01

The Koko Rift Zone (KRZ), eastern Oahu, is generally regarded as among the youngest volcanic features on the island. Previous workers have suggested that the 9 or 10 vents of this rift erupted near-simultaneously. However, K-Ar data in the literature (32-39 ka vs 320 ka) provide only general guidance on the youthfulness of these eruptions. We present new age constraints on KRZ volcanism using deposits of the phreatomagmatic eruption that produced Hanauma Bay (a popular snorkeling spot) and spatially associated lava flows. Numerous continuous basaltic ash units within the walls of Hanauma crater contain lithic fragments of well-preserved coral reef, beach rock, and marine mollusks, indicating that the eruption occurred in a near shore environment. 238U-234U-230Th dating of coral clasts in the deposit demonstrates that the eruption breached reef of MIS stage 7 age (200 +/- 30 ka), thereby ruling out the K-Ar age of 320 ka. U-series nuclides in "normal" MIS 7 coral lithics are indistinguishable from those in the island encircling Waianae Reef of the same age. However, U-series components in some originally aragonitic coral clasts were offset during the eruption when the rims recrystallized to calcite. 87Sr/86Sr, 234U/238U and Sr and U concentration indicate chemical mixing with host basaltic ash during this event, from which potential ages of the eruption can be constructed using isochron methods. More modeling of the data remains to be done but our preliminary estimate places the eruption at less than 100 ka. This result is consistent with new data on paleointensity and paleomagnetic secular variation within the lava flows exposed in or around the crater. This U-series dating approach should prove useful for eruptions in other locales where carbonate bioclast lithics are present in the deposits.

Action levels for airborne uranium in the workplace: chemical and radiological assessments.

PubMed

Leggett, R W; Meck, R A

2018-06-01

A method is described for deriving two levels of action-an investigation level (IL) and an immediate action level (IAL)-for different forms and mixtures of the natural uranium (U) isotopes 234 U, 235 U, and 238 U in air in the workplace. An IL indicates the need to confirm the validity of moderately elevated measurements of airborne U and adequacy of confinement controls and determine whether work limitations are appropriate. An IAL indicates that safeguards should be put into place immediately, including removal of workers from further exposure until conditions are acceptable. Derivations of ILs and IALs are based on latest radiation protection guidance, information on chemical toxicity of U, and biokinetic models for U. An action level (IL or IAL) is the more restrictive of two derived values, the action level based on U as a chemical hazard and the action level based on U as a radiation hazard.

NBL CRM 112-A: A new certified isotopic composition

NASA Astrophysics Data System (ADS)

Thomas, R. B.; Essex, R. M.; Mason, P.

2007-12-01

NBL CRM 112-A Uranium Metal Assay Standard is commonly used as a natural uranium isotopic reference material within the earth science mass spectrometry community. The metal is from the same parent material as NBS SRM 960, the uranyl nitrate solution, CRM 145, and the high-purity uranyl nitrate solution CRM 145-B. Because CRM 112-A has not yet been certified for isotopic composition, it has been assumed that this material has a natural 235U/238U (0.0072527), and the δ234U has been determined by measurement (e.g. -37.1‰; Cheng et al., 2000). These values have been widely used to calibrate the concentration of spikes and standards, and to correct measurements for instrument or mass bias. New, preliminary, isotopic measurements on CRM 145 and CRM 112-A performed at New Brunswick Laboratory suggest that these reference materials have a slightly lower 235U/238U and δ234U than have been commonly used. If this is the case, then data using the accepted values may be slightly biased. The significance of this bias will depend on the uncertainty of the measurement, how the CRM 112-A data is used to correct measurement data, the cited values that were used to correct the data, and the final certified values of the CRM. This fall, New Brunswick Laboratory is certifying the isotopic composition of the CRM 112-A metal using high precision thermal ionization mass spectrometry techniques. Upon completion of certification, the new CRM 112- A standard with certified isotopic ratios will provide the earth science community with a well characterized and traceable reference for calibrating and correcting their mass spectrometry measurement systems.

Depleted and enriched uranium exposure quantified in former factory workers and local residents of NL Industries, Colonie, NY USA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arnason, John G.

Background: Between 1958 and 1982, NL Industries manufactured components of enriched (EU) and depleted uranium (DU) at a factory in Colonie NY, USA. More than 5 metric tons of DU was deposited as microscopic DU oxide particles on the plant site and surrounding residential community. A prior study involving a small number of individuals (n=23) indicated some residents were exposed to DU and former workers to both DU and EU, most probably through inhalation of aerosol particles. Objectives: Our aim was to measure total uranium [U] and the uranium isotope ratios: {sup 234}U/{sup 238}U; {sup 235}U/{sup 238}U; and {sup 236}U/{supmore » 238}U, in the urine of a cohort of former workers and nearby residents of the NLI factory, to characterize individual exposure to natural uranium (NU), DU, and EU more than 3 decades after production ceased. Methods: We conducted a biomonitoring study in a larger cohort of 32 former workers and 99 residents, who may have been exposed during its period of operation, by measuring Total U, NU, DU, and EU in urine using Sector Field Inductively Coupled Plasma - Mass Spectrometry (SF-ICP-MS). Results: Among workers, 84% were exposed to DU, 9% to EU and DU, and 6% to natural uranium (NU) only. For those exposed to DU, urinary isotopic and [U] compositions result from binary mixing of NU and the DU plant feedstock. Among residents, 8% show evidence of DU exposure, whereas none shows evidence of EU exposure. For residents, the [U] geometric mean is significantly below the value reported for NHANES. There is no significant difference in [U] between exposed and unexposed residents, suggesting that [U] alone is not a reliable indicator of exposure to DU in this group. Conclusions: Ninety four percent of workers tested showed evidence of exposure to DU, EU or both, and were still excreting DU and EU decades after leaving the workforce. The study demonstrates the advantage of measuring multiple isotopic ratios (e.g., {sup 236}U/{sup 238}U and {sup 235}U/{sup 238}U) over a single ratio ({sup 235}U/{sup 238}U) in determining sources of uranium exposure. - Highlights: • Biomonitoring study of residents and former workers exposed to DU in Colonie NY. • Urine (99 residents+32 former workers) analyzed for depleted uranium (DU). • DU detected in 84% of workers and 8% of residents >30 years after plant closed. • Enriched uranium detected in 6% of former workers based on isotope ratios.« less

Uranium mobility across annual growth rings in three deciduous tree species

DOE Office of Scientific and Technical Information (OSTI.GOV)

McHugh, Kelly C.; Widom, Elisabeth; Spitz, Henry B.

Black walnut (Juglans nigra), slippery elm (Ulmus rubra), and white ash (Fraxinus americana) trees were evaluated as potential archives of past uranium (U) contamination. Like other metals, U mobility in annual growth rings of trees is potentially dependent on the tree species. Uranium concentrations and isotopic compositions (masses 234, 235, 236, and 238) were analyzed by thermal ionization mass spectrometry to test the efficacy of using tree rings to retroactively monitor U pollution from the FFMPC, a U purification facility operating from 1951 to 1989. This study found non-natural U (depleted U and detectable 236U) in growth rings of allmore » three tree species that pre-dated the start of operations at FFMPC and compositional trends that did not correspond with known contamination events. Therefore, the annual growth rings of these tree species cannot be used to reliably monitor the chronology of U contamination.« less

Uranium mobility across annual growth rings in three deciduous tree species.

PubMed

McHugh, Kelly C; Widom, Elisabeth; Spitz, Henry B; Wiles, Gregory C; Glover, Sam E

2018-02-01

Black walnut (Juglans nigra), slippery elm (Ulmus rubra), and white ash (Fraxinus americana) trees were evaluated as potential archives of past uranium (U) contamination. Like other metals, U mobility in annual growth rings of trees is dependent on the tree species. Uranium concentrations and isotopic compositions (masses 234, 235, 236, and 238) were analyzed by thermal ionization mass spectrometry to test the efficacy of using tree rings to retroactively monitor U pollution from the FFMPC, a U purification facility operating from 1951 to 1989. This study found non-natural U (depleted U and detectable 236 U) in growth rings of all three tree species that pre-dated the start of operations at FFMPC and compositional trends that did not correspond with known contamination events. Therefore, the annual growth rings of these tree species cannot be used to reliably monitor the chronology of U contamination. Copyright © 2017 Elsevier Ltd. All rights reserved.

Comparison of Grab, Air, and Surface Results for Radiation Site Characterization

NASA Astrophysics Data System (ADS)

Glassford, Eric Keith

2011-12-01

The use of proper sampling methods and sample types for evaluating sites believed to be contaminated with radioactive materials is necessary to avoid misrepresenting conditions at the site. This study was designed to investigate if the site characterization, based upon uranium contamination measured in different types of samples, is dependent upon the mass of the sample collected. A bulk sample of potentially contaminated interior dirt was collected from an abandoned metal processing mill that rolled uranium between 1948 and 1956. The original mill dates from 1910 and has a dirt floor. The bulk sample was a mixture of dirt, black and yellow particles of metal dust, and small fragments of natural debris. Small mass (approximately 0.75 grams (g)) and large mass (approximately 70g) grab samples were prepared from the bulk sample material to simulate collection of a "grab" type sample. Air sampling was performed by re-suspending a portion of the bulk sample material using a vibration table to simulate airborne contamination that might be present during site remediation. Additionally, samples of removable contaminated surface dust were collected on 47 mm diameter filter paper by wiping the surfaces of the exposure chamber used to resuspend the bulk material. Certified reference materials, one containing a precisely known quantity of U 3O8 and one containing a known quantity of natural uranium, were utilized to calibrate the gamma spectrometry measurement system. Non-destructive gamma spectrometry measurements were used to determine the content of uranium-235 (235U) at 185 keV and 143 keV, thorium-234 (234Th) at 63 keV, and protactinium-234m (234mPa) at 1001 keV in each sample. Measurement of natural uranium in small, 1 g samples is usually accomplished by radiochemical analysis in order to measure alpha particles emitted by 238U, 235U, and 234U. However, uranium in larger bulk samples can also be measured non-destructively using gamma spectrometry to detect the low energy photons from 234Th and 234mPa, the short-lived decay products of 238U, and 235U. Two sided t-tests and coefficient of variation were used to compare sampling types. The large grab samples had the lowest calculated coefficient of variation results for activity and atom percentage. The wipe samples had the highest calculated coefficient of variation of mean specific activity (dis/sec/g) for all three energies. The air filter samples had the highest coefficient of variation calculation for mean atom percentage, for both uranium isotopes examined. The data indicated that the large mass sample was the most effective at characterizing the rolling mill radioactive site conditions, since this would indicate which samples had the smallest variations compared to the mean. Additionally, measurement results of natural uranium in the samples indicate that the distribution of radioactive contamination at the sampling location is most likely non-homogeneous and that the size of the sample collected and analyzed must be sufficiently large to insure that the analytical results are truly representative of the activity present.

Estimation of uranium migration parameters in sandstone aquifers.

PubMed

Malov, A I

2016-03-01

The chemical composition and isotopes of carbon and uranium were investigated in groundwater samples that were collected from 16 wells and 2 sources in the Northern Dvina Basin, Northwest Russia. Across the dataset, the temperatures in the groundwater ranged from 3.6 to 6.9 °C, the pH ranged from 7.6 to 9.0, the Eh ranged from -137 to +128 mV, the total dissolved solids (TDS) ranged from 209 to 22,000 mg L(-1), and the dissolved oxygen (DO) ranged from 0 to 9.9 ppm. The (14)C activity ranged from 0 to 69.96 ± 0.69 percent modern carbon (pmC). The uranium content in the groundwater ranged from 0.006 to 16 ppb, and the (234)U:(238)U activity ratio ranged from 1.35 ± 0.21 to 8.61 ± 1.35. The uranium concentration and (234)U:(238)U activity ratio increased from the recharge area to the redox barrier; behind the barrier, the uranium content is minimal. The results were systematized by creating a conceptual model of the Northern Dvina Basin's hydrogeological system. The use of uranium isotope dating in conjunction with radiocarbon dating allowed the determination of important water-rock interaction parameters, such as the dissolution rate:recoil loss factor ratio Rd:p (a(-1)) and the uranium retardation factor:recoil loss factor ratio R:p in the aquifer. The (14)C age of the water was estimated to be between modern and >35,000 years. The (234)U-(238)U age of the water was estimated to be between 260 and 582,000 years. The Rd:p ratio decreases with increasing groundwater residence time in the aquifer from n × 10(-5) to n × 10(-7) a(-1). This finding is observed because the TDS increases in that direction from 0.2 to 9 g L(-1), and accordingly, the mineral saturation indices increase. Relatively high values of R:p (200-1000) characterize aquifers in sandy-clayey sediments from the Late Pleistocene and the deepest parts of the Vendian strata. In samples from the sandstones of the upper part of the Vendian strata, the R:p value is ∼ 24, i.e., sorption processes are expressed more weakly, and uranium is possibly desorbed from the sediments. Overall, these results provide a better understanding of the evolution of uranium isotopes in groundwater systems. Copyright © 2015 Elsevier Ltd. All rights reserved.

Isotopic tracing of the dissolved U fluxes of Himalayan rivers: implications for present and past U budgets of the Ganges-Brahmaputra system

NASA Astrophysics Data System (ADS)

Chabaux, François; Riotte, Jean; Clauer, Norbert; France-Lanord, Christian

2001-10-01

U activity ratios have been measured in the dissolved loads of selected rivers from the Himalayan range, in Central Nepal, and from the Bangladesh, as well as in some rain waters. A few European and Asian rivers have also been analyzed for their U activity ratios. The data confirm the negligible effect of rainwater on the budget of dissolved U in river waters. The results also indicate that rivers on each Himalayan structural unit have homogeneous and specific U isotope compositions: i) (234U/238U) activity ratios slightly lower than unity in the dissolved load of the streams draining the Tethyan Sedimentary Series (TSS); ii) values slightly higher than unity for waters from the High Himalaya Crystalline (HHC) and the Lesser Himalaya (LH); iii) systematically higher (234U/238U) activity ratios for waters from the Siwaliks. Thus, U activity ratios, in association with Sr isotopic ratios, can be used to trace the sources of dissolved fluxes carried by these rivers. Coupling of U with Sr isotope data shows (1) that the U carried by the dissolved load of the Himalayan rivers mainly originates from U-rich lithologies of the TSS in the northern formations of the Tibetan plateau; and (2) that the elemental U and Sr fluxes carried by the Himalayan rivers at the outflow of the highlands are fairly homogeneous at the scale of the Himalayan chain. Rivers flowing on the Indian plain define a different trend from that of the Himalayan rivers in the U-Sr isotopic diagram, indicating the contribution of a specific floodplain component to the U and Sr budgets of the Ganges and the Brahmaputra. The influence of this component remains limited to 10 to 15 percent for the U flux, but can contribute 35 to 55% of the Sr flux. The variations of the Sr and U fluxes of the Ganges-Brahmaputra river system in response to climatic variations have been estimated by assuming a temporary cut off of the chemical fluxes from high-altitude terrains during glacial episodes. This scenario would significantly decrease the dissolved U flux of the Ganges-Brahmaputra river system and increase its U activity ratio. Such a climatic dependence of the Himalayan U flux could induce a periodic variation of the mean U activity ratio of the world rivers on glacial-interglacial timescales

Tracing Anthropogenic Salinity Inputs to the Semi-arid Rio Grande River: A Multi-isotope Tracer (U, S, B and Sr) Approach

NASA Astrophysics Data System (ADS)

Garcia, S.; Nyachoti, S. K.; Ma, L.; Szynkiewicz, A.; McIntosh, J. C.

2015-12-01

High salinity in the Rio Grande has led to severe reductions in crop productivity and accumulation of salts in soils. These pressing issues exist for other arid rivers worldwide. Salinity contributions to the Rio Grande have not been adequately quantified, especially from agriculture, urban activities, and geological sources. Here, we use major element concentrations and U, S, B, Sr isotopic signatures to fingerprint the salinity sources. Our study area focuses on a 200 km long stretch of the Rio Grande from Elephant Butte Reservoir, NM to El Paso, TX. River samples were collected monthly from 2014 to 2015. Irrigation drains, groundwater wells, city drains and wastewater effluents were sampled as possible anthropogenic salinity end-members. Major element chemistry, U, S and Sr isotope ratios in the Rio Grande waters suggest multiple salinity inputs from geological, agricultural, and urban sources. Natural upwelling of groundwater is significant for the Rio Grande near Elephant Butte, as suggested by high TDS values and high (234U/238U), 87Sr/86Sr, δ34S ratios. Agricultural activities (e.g. flood irrigation, groundwater pumping, fertilizer use) are extensive in the Mesilla Valley. Rio Grande waters from this region have characteristic lower (234U/238U), 87Sr/86Sr, and δ34S ratios, with possible agricultural sources from use of fertilizers and gypsum. Agricultural practices during flood irrigation also intensify evaporation of Rio Grande surface water and considerably increase water salinity. Shallow groundwater signatures were also identified at several river locations, possibly due to the artificial pumping of local groundwater for irrigation. Impacts of urban activities to river chemistry (high NO3 and B concentrations) were evident for locations downstream to Las Cruces and El Paso wastewater treatment plants, supporting the use of the B isotope as an urban salinity tracer. This study improves our understanding of human impacts on water quality and elemental cycles.

234U/238U and δ87Sr in peat as tracers of paleosalinity in the Sacramento-San Joaquin Delta of California, USA

USGS Publications Warehouse

Drexler, Judith Z.; Paces, James B.; Alpers, Charles N.; Windham-Myers, Lisamarie; Neymark, Leonid; Bullen, Thomas D.; Taylor, Howard E.

2013-01-01

The purpose of this study was to determine the history of paleosalinity over the past 6000+ years in the Sacramento-San Joaquin Delta (the Delta), which is the innermost part of the San Francisco Estuary. We used a combination of Sr and U concentrations, d87Sr values, and 234U/238U activity ratios (AR) in peat as proxies for tracking paleosalinity. Peat cores were collected in marshes on Browns Island, Franks Wetland, and Bacon Channel Island in the Delta. Cores were dated using 137Cs, the onset of Pb and Hg contamination from hydraulic gold mining, and 14C. A proof of concept study showed that the dominant emergent macrophyte and major component of peat in the Delta, Schoenoplectus spp., incorporates Sr and U and that the isotopic composition of these elements tracks the ambient water salinity across the Estuary. Concentrations and isotopic compositions of Sr and U in the three main water sources contributing to the Delta (seawater, Sacramento River water, and San Joaquin River water) were used to construct a three-end-member mixing model. Delta paleosalinity was determined by examining variations in the distribution of peat samples through time within the area delineated by the mixing model. The Delta has long been considered a tidal freshwater marsh region, but only peat samples from Franks Wetland and Bacon Channel Island have shown a consistently fresh signal (<0.5 ppt) through time. Therefore, the eastern Delta, which occurs upstream from Bacon Channel Island along the San Joaquin River and its tributaries, has also been fresh for this time period. Over the past 6000+ years, the salinity regime at the western boundary of the Delta (Browns Island) has alternated between fresh and oligohaline (0.5-5 ppt).

Diagenesis of fossil coral skeletons: Correlation between trace elements, textures, and [sup 234]U/[sup 238]U

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bar-Matthews, M.; Wasserburg, G.J.; Chen, J.H.

1993-01-01

A comparative study of Pleistocene fossil coral skeletons and of modern coral skeletons was carried out using petrographic and trace element analyses on a suite of Pleistocene samples that had previously been studied from [sup 234]U, [sup 230]Th, and U-[sup 230]Th ages (Chen et al. 1991). Evidence of a range of diagenetic changes can be recognized by optical (OM) and scanning electron microscopy (SEM). Using an electron microprobe and SEM, concentrations of Na, S, Sr, and Mg were measured. No other trace elements were detected. Na, S, and Mg contents of the matrix, the fibrous micropores, and radiating needles aremore » highly variable and well correlated. High concentrations of Na, S, and Mg were found in modern living corals with lower concentrations in fossil corals and fibrous micropores, and the lowest value in the radiating needles. The reason for the correlations of Na, S, and Mg and crystal chemistry and the response to diagenesis of these trace elements is not understood. The average concentrations of Na, S, and Mg for each sample, when plotted against the whole coral initial [delta][sup 234]U, are generally correlated (Chen et al., 1991). As all these diagenetic changes involve the recystallization and deposition of aragonite, the authors infer that the geologic site of diagenesis both for forming the secondary aragonitic phases and for the enhancement of the [sup 234]U content in the fossil corals was the marine environment. It is possible that the textural and Na, S, and Mg trace element contents of fossil corals be used to ascertain the reliability of fossil coral skeletons for U-[sup 230]Th dating. The basic problem of identifying a priori unaltered coral skeletons for [sup 230]Th dating is not yet resolved. 64 refs., 16 figs., 5 tabs.« less

Isotope hydrology of the Chalk River Laboratories site, Ontario, Canada

USGS Publications Warehouse

Peterman, Zell; Neymark, Leonid; King-Sharp, K.J.; Gascoyne, Mel

2016-01-01

This paper presents results of hydrochemical and isotopic analyses of groundwater (fracture water) and porewater, and physical property and water content measurements of bedrock core at the Chalk River Laboratories (CRL) site in Ontario. Density and water contents were determined and water-loss porosity values were calculated for core samples. Average and standard deviations of density and water-loss porosity of 50 core samples from four boreholes are 2.73 ± 12 g/cc and 1.32 ± 1.24 percent. Respective median values are 2.68 and 0.83 indicating a positive skewness in the distributions. Groundwater samples from four deep boreholes were analyzed for strontium (87Sr/86Sr) and uranium (234U/238U) isotope ratios. Oxygen and hydrogen isotope analyses and selected solute concentrations determined by CRL are included for comparison. Groundwater from borehole CRG-1 in a zone between approximately +60 and −240 m elevation is relatively depleted in δ18O and δ2H perhaps reflecting a slug of water recharged during colder climatic conditions. Porewater was extracted from core samples by centrifugation and analyzed for major dissolved ions and for strontium and uranium isotopes. On average, the extracted water contains 15 times larger concentration of solutes than the groundwater. 234U/238U and correlation of 87Sr/86Sr with Rb/Sr values indicate that the porewater may be substantially older than the groundwater. Results of this study show that the Precambrian gneisses at Chalk River are similar in physical properties and hydrochemical aspects to crystalline rocks being considered for the construction of nuclear waste repositories in other regions.

Solid-phase data from cores at the proposed Dewey Burdock uranium in-situ recovery mine, near Edgemont, South Dakota

USGS Publications Warehouse

Johnson, Raymond H.; Diehl, Sharon F.; Benzel, William M.

2013-01-01

This report releases solid-phase data from cores at the proposed Dewey Burdock uranium in-situ recovery site near Edgemont, South Dakota. These cores were collected by Powertech Uranium Corporation, and material not used for their analyses were given to the U.S. Geological Survey for additional sampling and analyses. These additional analyses included total carbon and sulfur, whole rock acid digestion for major and trace elements, 234U/238U activity ratios, X-ray diffraction, thin sections, scanning electron microscopy analyses, and cathodoluminescence. This report provides the methods and data results from these analyses along with a short summary of observations.

Thorium-234 as a tracer of spatial, temporal and vertical variability in particle flux in the North Pacific

NASA Astrophysics Data System (ADS)

Buesseler, K. O.; Pike, S.; Maiti, K.; Lamborg, C. H.; Siegel, D. A.; Trull, T. W.

2009-07-01

An extensive 234Th data set was collected at two sites in the North Pacific: ALOHA, an oligotrophic site near Hawaii, and K2, a mesotrophic HNLC site in the NW Pacific as part of the VERTIGO (VERtical Transport In the Global Ocean) study. Total 234Th: 238U activity ratios near 1.0 indicated low particle fluxes at ALOHA, while 234Th: 238U ˜0.6 in the euphotic zone at K2 indicated higher particle export. However, spatial variability was large at both sites—even greater than seasonal variability as reported in prior studies. This variability in space and time confounds the use of single profiles of 234Th for sediment trap calibration purposes. At K2, there was a decrease in export flux and increase in 234Th activities over time associated with the declining phase of a summer diatom bloom, which required the use of non-steady state models for flux predictions. This variability in space and time confounds the use of single profiles of 234Th for sediment trap calibration purposes. High vertical resolution profiles show narrow layers (20-30 m) of excess 234Th below the deep chlorophyll maximum at K2 associated with particle remineralization resulting in a decrease in flux at depth that may be missed with standard sampling for 234Th and/or with sediment traps. Also, the application of 234Th as POC flux tracer relies on accurate sampling of particulate POC/ 234Th ratios and here the ratio is similar on sinking particles and mid-sized particles collected by in-situ filtration (>10-50 μm at ALOHA and >5-350 μm at K2). To further address variability in particle fluxes at K2, a simple model of the drawdown of 234Th and nutrients is used to demonstrate that while coupled during export, their ratios in the water column will vary with time and depth after export. Overall these 234Th data provide a detailed view into particle flux and remineralization in the North Pacific over time and space scales that are varying over days to weeks, and 10's-100's km at a resolution that is difficult to obtain with other methods.

Fluxes of 238U decay series radionuclides in a dicalcium phosphate industrial plant.

PubMed

Casacuberta, N; Masqué, P; Garcia-Orellana, J

2011-06-15

The production of dicalcium phosphate (DCP) is part of the phosphate industry, which has been recently included in the positive list of the NORM industries defined in the revised version of the EU-BSS (Euratom 29/96). The objective of the present work is to study specific concentrations and fluxes of (238,234)U, (230)Th, (226)Ra, (210)Pb and (210)Po at the different stages of the DCP production. Results showed highest activities of (238)U and (210)Pb were found in DCP (1500-2000 Bq kg(-1)); (230)Th and (210)Po were released together with the sludges (1600-2000 Bq kg(-1)) and (226)Ra presented particularly high activities in water (48 × 10(3) Bq m(-3)) and in the reactor scales (115 × 10(3) Bq kg(-1)). Fluxes of radionuclides showed that (238)U outflows were equally distributed between sludges (16 × 10(3) kBq h(-1)) and dicalcium phosphate (20 × 10(3) kBq h(-1)); (230)Th and (210)Po were almost entirely released in the sludges (30 × 10(3)kBq h(-1)) and the greatest (210)Pb outflow was the DCP current (25 × 10(3) kBq h(-1)). (226)Ra was mainly discharged through the water effluent (12 × 10(3) kBq h(-1)). This work highlights the importance of studying the industrial processes involving NORM, as minor changes in the production steps lead to different radionuclide distribution in the process. Copyright © 2011 Elsevier B.V. All rights reserved.

The application of U-isotopes to assess weathering in contrasted soil-water regime in Brazil.

PubMed

Rosolen, Vania; Bueno, Guilherme Taitson; Bonotto, Daniel Marcos

2018-02-01

This paper presents the use of U-series radionuclides 238 U and 234 U to evaluate the biogeochemical disequilibrium in soil cover under a contrasted soil-water regime. The approach was applied in three profiles located in distinct topographical positions, from upslope ferralitic to downslope hydromorphic domain. The U fractionation data was obtained in the samples representing the saprolite and the superficial and subsuperficial soil horizons. The results showed a significant and positive correlation between U and the Total Organic Carbon (TOC). Soil organic matter has accumulated in soil due to hydromorphy. There is no evidence of positive correlation between U and Fe, as expected in lateritic soils. The advance of the hydromorphy on Ferralsol changes the weathering rates, and the ages of weathering are discussed as a function of the advance of waterlogged soil conditions from downslope. Also, the bioturbation could represent the other factor responsible to construct a more recent soil horizon. Copyright © 2017 Elsevier Ltd. All rights reserved.

A review of the high temperature oxidation of uranium oxides in molten salts and in the solid state to form alkali metal uranates, and their composition and properties

NASA Astrophysics Data System (ADS)

Griffiths, Trevor R.; Volkovich, Vladimir A.

An extensive review of the literature on the high temperature reactions (both in melts and in the solid state) of uranium oxides (UO 2, U 3O 8 and UO 3) resulting in the formation of insoluble alkali metal (Li to Cs) uranates is presented. Their uranate(VI) and uranate(V) compounds are examined, together with mixed and oxygen-deficient uranates. The reactions of uranium oxides with carbonates, oxides, per- and superoxides, chlorides, sulfates, nitrates and nitrites under both oxidising and non-oxidising conditions are critically examined and systematised, and the established compositions of a range of uranate(VI) and (V) compounds formed are discussed. Alkali metal uranates(VI) are examined in detail and their structural, physical, thermodynamic and spectroscopic properties considered. Chemical properties of alkali metal uranates(VI), including various methods for their reduction, are also reported. Errors in the current theoretical treatment of uranate(VI) spectra are identified and the need to develop routes for the preparation of single crystals is stressed.

The chronology for the d18O record from Devils Hole, Nevada, extended into the Mid-Holocene

USGS Publications Warehouse

Landwehr, J.M.; Sharp, W.D.; Coplen, T.B.; Ludwig, K. R.; Winograd, I.J.

2011-01-01

This report presents the numeric values for the chronology of the paleoclimatically relevant mid-to-late Pleistocene record of the ratios of stable oxygen isotope (delta18O) in vein calcite from Devils Hole, Nev., which recently had been extended into the mid-Holocene. Dating was obtained using 230Th-234U-238U thermal ionization mass spectrometry. Devils Hole is a subaqueous cave of tectonic origin, which developed in the discharge zone of a regional aquifer in south-central Nevada. The primary groundwater recharge source area is the Spring Mountains, the highest mountain range in southern Nevada [altitude 3,630 meters (m)], approximately 80 kilometers to the east of the cavern. The walls of the open fault zone comprising the cave system are coated with dense vein calcite precipitated from the through-flowing groundwater. The calcite, up to 40 centimeters (cm) thick, contains a continuous record of the sequential variation of the composition of stable oxygen isotopes in the ground water over time. The vein calcite has also proven to be a suitable material for precise uranium-series dating via thermal ionization mass spectrometry utilizing the 230Th-234U-238U decay clock. Earlier work has presented data from the Devils Hole core DH-11, a 36-cm-long core of vein calcite recovered from a depth of about 30 m below the water table (about 45 m beneath the ground surface). The DH-11 core provided a continuous record of isotopic oxygen variation from 567,700 to 59,800 years before present. Recent work has extended this record up to 4,500 years before present, into the mid-Holocene epoch.

Meta-analysis of depleted uranium levels in the Middle East region.

PubMed

Bešić, Larisa; Muhović, Imer; Mrkulić, Fatima; Spahić, Lemana; Omanović, Ammar; Kurtovic-Kozaric, Amina

2018-06-08

Since the first widespread use of depleted uranium in military in the 1991 Gulf War, the so-called "Gulf War Syndrome" has been a topic of ongoing debate. However, a low number of reliable scientific papers demonstrating the extent of possible contamination as well as its connection to the health status of residents and deployed veterans has been published. The authors of this study have therefore aimed to make a selection of data based on strict inclusion and exclusion criteria. With the goal of clarifying the extent of DU contamination after the Gulf Wars, previously published data regarding the levels of DU in the Middle East region were analyzed and presented in the form of a meta-analysis. In addition, the authors attempted to make a correlation between the DU levels and their possible effects on afflicted populations. According to results observed by comparing 234 U/ 238 U and 235 U/ 238 U isotopic activity ratios, as well as 235 U/ 238 U mass ratios in air, water, soil and food samples among the countries in the Middle East region, areas indicating contamination with DU were Al Doha, Manageesh and Um Al Kwaty in Kuwait, Al-Salman, Al-Nukhaib and Karbala in Iraq, Beirut in Lebanon and Sinai in Egypt. According to these data, no DU contamination was observed in Algeria, Israel, Afghanistan, Oman, Qatar, Iran, and Yemen. Due to the limited number of reliable data on the health status of afflicted populations, it was not possible to make a correlation between DU levels and health effects in the Middle East region. Copyright © 2018. Published by Elsevier Ltd.

Concentrations of selected radionuclides and their spatial distribution in marine sediments from the northwestern Gulf, Kuwait.

PubMed

Uddin, Saif; Behbehani, Montaha

2018-02-01

This study focuses on creating a baseline for 40 K, 210 Pb, 137 Cs, 90 Sr, 226 Ra, 228 Ra, 238 U, 235 U, 234 U, 239+240 Pu and 238 Pu in marine sediments in the northwestern Gulf. The respective measured concentration ranges were 386-489, 32.3-48.8, 1.5-2.9, 4.53-5.42, 18.3-23.1, 18.8-23.0, 22.3-30.5, 0.99-1.33, 25.6-34.8, 0.30-0.93, and 0.0008-0.00018Bqkg -1 . The levels of these radionuclides are generally comparable to values reported for other marine waters in the northern hemisphere. The 137 Cs activity in the Gulf sediments offshore Kuwait is an order of magnitude lower compared to sediments from northeastern Iran. Other than that finding, no hot spots were observed in sediments adjacent to power and desalination plants, oil and gas industrial activities or wastewater treatment facilities. These data will serve as a baseline to gauge possible future inputs of radionuclides in the northern Gulf. The calculated average ratio of 235 U/ 238 U activity in the area is in agreement with the reported figure of the natural uranium ratio, suggesting the absence of depleted uranium (DU) at all the stations. The low concentration of 239+240 Pu suggests that there is no significant source of plutonium except that from atmospheric fallout from weapon testing and possible dry deposition via long-range dust transport. Copyright © 2017 Elsevier Ltd. All rights reserved.

Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV).

PubMed

Jemison, Noah E; Shiel, Alyssa E; Johnson, Thomas M; Lundstrom, Craig C; Long, Philip E; Williams, Kenneth H

2018-03-20

Biostimulation to induce reduction of soluble U(VI) to relatively immobile U(IV) is an effective strategy for decreasing aqueous U(VI) concentrations in contaminated groundwater systems. If oxidation of U(IV) occurs following the biostimulation phase, U(VI) concentrations increase, challenging the long-term effectiveness of this technique. However, detecting U(IV) oxidation through dissolved U concentrations alone can prove difficult in locations with few groundwater wells to track the addition of U to a mass of groundwater. We propose the 238 U/ 235 U ratio of aqueous U as an independent, reliable tracer of U(IV) remobilization via oxidation or mobilization of colloids. Reduction of U(VI) produces 238 U-enriched U(IV), whereas remobilization of solid U(IV) should not induce isotopic fractionation. The incorporation of remobilized U(IV) with a high 238 U/ 235 U ratio into the aqueous U(VI) pool produces an increase in 238 U/ 235 U of aqueous U(VI). During several injections of nitrate to induce U(IV) oxidation, 238 U/ 235 U consistently increased, suggesting 238 U/ 235 U is broadly applicable for detecting mobilization of U(IV).

Combined uranous nitrate production consisting of undivided electrolytic cell and divided electrolytic cell (Electrolysis → Electrolytic cell)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yuan, Zhongwei; Yan, Taihong; Zheng, Weifang

2013-07-01

The electrochemical reduction of uranyl nitrate is a green, mild way to make uranous ions. Undivided electrolyzers whose maintenance is less but their conversion ratio and current efficiency are low, have been chosen. However, at the beginning of undivided electrolysis, high current efficiency can also be maintained. Divided electrolyzers' conversion ratio and current efficiency is much higher because the re-oxidation of uranous on anode is avoided, but their maintenance costs are more, because in radioactive environment the membrane has to be changed after several operations. In this paper, a combined method of uranous production is proposed which consists of 2more » stages: undivided electrolysis (early stage) and divided electrolysis (late stage) to benefit from the advantages of both electrolysis modes. The performance of the combined method was tested. The results show that in combined mode, after 200 min long electrolysis (80 min undivided electrolysis and 120 min divided electrolysis), U(IV) yield can achieve 92.3% (500 ml feed, U 199 g/l, 72 cm{sup 2} cathode, 120 mA/cm{sup 2}). Compared with divided mode, about 1/3 working time in divided electrolyzer is reduced to achieve the same U(IV) yield. If 120 min long undivided electrolysis was taken, more than 1/2 working time can be reduced in divided electrolyzer, which means that about half of the maintenance cost can also be reduced. (authors)« less

Plutonium and uranium in human bones from areas surrounding the Semipalatinsk nuclear test site.

PubMed

Yamamoto, Masayoshi; Hoshi, Masaharu; Sakaguchi, Aya; Shinohara, Kunihiko; Kurihara, Osamu; Apsalikov, Kazbek N; Gusev, Boris I

2006-02-01

To evaluate the present levels of 239,240Pu and U in residents living near the Semipalatinsk nuclear test site, more than 70 bone samples were obtained at autopsy. The subjects ranged in age from 30 to 86 years (mean 59.3+/-12.9). Most of the samples consisted of victims who died of various diseases. Plutonium and U were radiochemically separated and determined by alpha-ray spectrometry. The mean concentrations of 239,240Pu and 238U observed were 0.050+/-0.041 mBq/g-ash (vertebrae 71, long-bones 18) and 0.28+/-0.13 mBq/g-ash (22.8+/-10.6 microg U/kg-ash) (vertebrae 58, long bones 16), respectively. The present 239,240Pu levels were within the range found for human bone samples from other countries due solely to global fallout in the early 1980s. The average U concentration was close to the estimate (mean 22.5 microg U/kg-ash) for the UK, and about 10 times higher than those estimated for residents in New York City and Japan. By assuming that the average concentration of 239,240Pu in bone samples is the value at 45 years after instantaneous inhalation in 1955, the initial total intake and the effective dose for 45 years were estimated as 10 Bq and 0.2 mSv, respectively. The annual intake of total U (234,235,238U) and its effective dose for 60 years were estimated as 30 Bq for adult and 0.1 mSv, respectively, for chronic ingestion.

Measuring U-series Disequilibrium in Weathering Rinds to Study the Influence of Environmental Factors to Weathering Rates in Tropical Basse-Terre Island (French Guadeloupe)

NASA Astrophysics Data System (ADS)

Guo, J.; Ma, L.; Sak, P. B.; Gaillardet, J.; Chabaux, F. J.; Brantley, S. L.

2015-12-01

Chemical weathering is a critical process to global CO2 consumption, river/ocean chemistry, and nutrient import to biosphere. Weathering rinds experience minimal physical erosion and provide a well-constrained system to study the chemical weathering process. Here, we applied U-series disequilibrium dating method to study weathering advance rates on the wet side of Basse-Terre Island, French Guadeloupe, aiming to understand the role of the precipitation in controlling weathering rates and elucidate the behavior and immobilization mechanisms of U-series isotopes during rind formation. Six weathering clasts from 5 watersheds with mean annual precipitation varying from 2000 to 3000 mm/yr were measured for U-series isotope ratios and major element compositions on linear core-to-rind transects. One sample experienced complete core-to-rind transformation, while the rest clasts contain both rinds and unweathered cores. Our results show that the unweathered cores are under U-series secular equilibrium, while all the rind materials show significant U-series disequilibrium. For most rinds, linear core-to-rind increases of (230Th/232Th) activity ratios suggest a simple continuous U addition history. However, (234U/238U) and (238U/232Th) trends in several clasts show evidences of remobilization of Uranium besides the U addition, complicating the use of U-series dating method. The similarity between U/Th ratios and major elements trends like Fe, Al, P in some transects and the ongoing leaching experiments suggest that redox and organic colloids could control the mobilization of U-series isotopes in the rinds. Rind formation ages and weathering advance rate (0.07-0.29mm/kyr) were calculated for those rinds with a simple U-addition history. Our preliminary results show that local precipitation gradient significantly influenced the weathering advance rate, revealing the potential of estimating weathering advance rates at a large spatial scale using the U-series dating method.

Measurement of the 234U(n, f ) cross-section with quasi-monoenergetic beams in the keV and MeV range using a Micromegas detector assembly

NASA Astrophysics Data System (ADS)

Stamatopoulos, A.; Kanellakopoulos, A.; Kalamara, A.; Diakaki, M.; Tsinganis, A.; Kokkoris, M.; Michalopoulou, V.; Axiotis, M.; Lagoyiannis, A.; Vlastou, R.

2018-01-01

The 234U neutron-induced fission cross-section has been measured at incident neutron energies of 452, 550, 651 keV and 7.5, 8.7, 10 MeV using the 7Li ( p, n) and the 2H( d, n) reactions, respectively, relative to the 235U( n, f ) and 238U( n, f ) reference reactions. The measurement was performed at the neutron beam facility of the National Center for Scientific Research "Demokritos", using a set-up based on Micromegas detectors. The active mass of the actinide samples and the corresponding impurities were determined via α-spectroscopy using a surface barrier silicon detector. The neutron spectra intercepted by the actinide samples have been thoroughly studied by coupling the NeuSDesc and MCNP5 codes, taking into account the energy and angular straggling of the primary ion beams in the neutron source targets in addition to contributions from competing reactions ( e.g. deuteron break-up) and neutron scattering in the surrounding materials. Auxiliary Monte Carlo simulations were performed making combined use of the FLUKA and GEF codes, focusing particularly on the determination of the fission fragment detection efficiency. The developed methodology and the final results are presented.

Fractionation of 238U/235U by reduction during low temperature uranium mineralisation processes

NASA Astrophysics Data System (ADS)

Murphy, Melissa J.; Stirling, Claudine H.; Kaltenbach, Angela; Turner, Simon P.; Schaefer, Bruce F.

2014-02-01

Investigations of ‘stable’ uranium isotope fractionation during low temperature, redox transformations may provide new insights into the usefulness of the 238U/235U isotope system as a tracer of palaeoredox processes. Sandstone-hosted uranium deposits accumulate at an oxidation/reduction interface within an aquifer from the low temperature reduction of soluble U(VI) complexes in groundwaters, forming insoluble U(IV) minerals. This setting provides an ideal environment in which to investigate the effects of redox transformations on 238U/235U fractionation. Here we present the first coupled measurements of 238U/235U isotopic compositions and U concentrations for groundwaters and mineralised sediment samples from the same redox system in the vicinity of the high-grade Pepegoona sandstone-hosted uranium deposit, Australia. The mineralised sediment samples display extremely variable 238U/235U ratios (herein expressed as δUCRM145238, the per-mil deviation from the international NBL standard CRM145). The majority of mineralised sediment samples have δUCRM145238 values between -1.30±0.05 and 0.55±0.12‰, spanning a ca. 2‰ range. However, one sample has an unusually light isotopic composition of -4.13±0.05‰, which suggests a total range of U isotopic variability of up to ca. 5‰, the largest variation found thus far in a single natural redox system. The 238U/235U isotopic signature of the mineralised sediments becomes progressively heavier (enriched in 238U) along the groundwater flow path. The groundwaters show a greater than 2‰ variation in their 238U/235U ratios, ranging from δUCRM145238 values of -2.39±0.07 to -0.71±0.05‰. The majority of the groundwater data exhibit a clear systematic relationship between 238U/235U isotopic composition and U concentration; samples with the lowest U concentrations have the lowest 238U/235U ratios. The preferential incorporation of 238U during reduction of U(VI) to U(IV) and precipitation of uranium minerals leaves the groundwaters enriched in 235U, resulting in a progressive shift in 238U/235U towards lighter values in the aqueous phase as U is removed. These data can be modelled by a closed system Rayleigh fractionation model, with a fractionation factor (α, representing the 238U/235U composition of the groundwater relative to the solid uranium minerals) ranging from ∼0.9996 to 1.0000, with the majority of datapoints ranging from α values of 0.9998 to 0.9999. The sense and magnitude of the results of this study imply that 238U/235U fractionation is likely to be controlled by volume-dependent nuclear field shift effects during the reduction of U(VI) to U(IV) during mineralisation processes. These findings support the use of the 238U/235U isotopic system as a tracer to constrain the nature and timing of palaeoredox conditions.

Uranium and Its Decay Products in Floodplain Sediments from the River Fal

NASA Astrophysics Data System (ADS)

Millward, G. E.; Blake, W. H.; Little, R.; Couldrick, L.

2012-04-01

European river basins are subject to longer-term storage of legacy contaminants in sedimentary sinks and their potential release presents a credible risk to achieving water quality targets required by the EU Water Framework Directive. The catchment of the River Fal, south west England, is extensively mineralised and has been greatly impacted by heavy metal mining. Uranium and radium were extracted and processed between 1870 and 1930 and spoil tips along the channel banks are assumed to have been a source of radionuclides into the river. Radionuclides were determined in five cores obtained from the river floodplain, including a reference core positioned upstream of the uranium mine enabling evaluation of its impact on past and contemporary sediment quality. The core was sectioned into 1 cm thick slices and they were analysed by gamma spectrometry for products of the U-238 decay series, i.e. Th-234 (a surrogate for U-238), Pb-214 (a surrogate for Ra-226), Pb-210 and fallout Am-241 and Cs-137. Peak Cs-137 concentrations at mid-depth were associated with fallout after atmospheric nuclear tests in 1963 and were used to estimate sedimentation rates. However, the activity concentrations of Pb-210 were elevated at all depths and the result indicated a significant input of unsupported Pb-210 (linked to processed spoil material) throughout the period of deposition. At some sites, peak activity concentrations of Th-234 suggested inputs from mining activity during major release and/or flood events. The cores downstream of the mine all had higher radionuclide inventories, of the order 105 Bq m-2, compared to the reference core due to the presences of products from the U-238 decay series. In addition, the inventories did not decrease systematically downstream indicating storage regions within the river channel. Storage of such legacy contaminants at levels in excess of contemporary environmental quality guidelines raises important questions and challenges for floodplain use and management.

Testing the Limits to Accurate Comminution Dates: A Progress Report

NASA Astrophysics Data System (ADS)

Piccione, G.; Blackburn, T.; Edwards, G. H.

2017-12-01

The ability to resolve the timing of fine particle production holds potential for contributing to several Earth Science sub-disciplines including glaciology, eolian and fluvial geomorphology, soil production, and fault dynamics. A relatively new geochronologic tool, U-series comminution dating, has shown potential to directly date the timing of particle comminution. This system's sensitivity to particle size arises from a physical disequilibrium in the 238U decay chain generated by the ejected loss of intermediate daughter products (e.g. 234U). It is the goal of this ongoing study to develop and test analytical procedures to improve the accuracy of comminution dating. In the geologic settings explored by previous studies, comminution dates integrate both the time of particle transport and time since deposition. To better test the accuracy of comminution dates, our study focuses on settings where silt has experienced little to no transport time, specifically, glacial moraines in the Eastern Sierras and Rock Avalanches in the San Gabriel Mountains, both locations with existing independent geochronologic constraints. Previous studies demonstrate the dependency of U-series comminution date on grain size and shape. Here we show that mineralogy of samples also plays a role, possibly controlled by the uranium content and crystal bond strength. To separate samples by size and mineralogy, we use dry sonic-sieving, density and magnetic separation. Non-detrital materials deposited on the rim of comminuted grains have an isotopic composition that is unrelated to the isotopic evolution since comminution and therefore must be removed through a multi-step leaching procedure. Leaching is complicated by the fact that areas within the comminuted crystal that have experienced physical fractionation are contained within damaged zones and are prone to being leached themselves, which removes areas of interest from the crystal. We present progress made on a sample processing method developed to alleviate complications that affect comminution age measurements. Initial 234U/238U measurements for untreated silt from an 800ka Sierran glacial till are up to 6% above secular equilibrium, while samples processed with this method have measured ratios as low as 3% below secular equilibrium.

The Application of 238U/235U as a Redox-Proxy for Past Ocean Chemistry

NASA Astrophysics Data System (ADS)

Andersen, M. B.; Westermann, S.; Bahniuk, A.; Vasconcelos, C.; McKenzie, J. A.; Föllmi, K. B.; Vance, D.

2014-12-01

The recent discovery of significant variation in 238U/235U caused by redox change at the surface Earth has led to its use to extract information on the oxygenation state of ancient oceans from marine sediments [e.g. 1]. Recent studies have focused on improving the understanding of the 238U/235U signature in modern marine carbonates [2] and black shales [3] to improve the robustness of this tracer. To further advance its use we have focused on improving our understanding of 238U/235U systematics in modern dolomite, another commonly occurring rock-type in the geological record, before turning to 238U/235U signatures in ancient sediments. The measured dolomite samples, precipitated in modern environments of coastal hypersaline lagoons in Brazil, all exhibit 238U/235U values that deviate from the seawater composition [3]. Observed values are both lighter (ca. 130 ppm; as also observed in dolomite from tidal-ponds on Bahamas [2]) and heavier (50-180 ppm). These distinct 238U/235U values for different dolomite-precipitates likely attest to the particular formation style, as well as early diagenetic processes. We use such modern settings to discuss the utility of 238U/235U in ancient sediments, the singularity of any observed 238U/235U signal, its relation to global ocean chemistry and potential diagenetic overprinting. These constraints are then used to evaluate a well-preserved marine carbonate section [4] and published black shale 238U/235U data [1], both deposited during the Oceanic Anoxic Event 2 (93 Ma). We discuss the capabilities of both the carbonate and black shale section for retaining information on the 238U/235U composition in the ocean during OAE 2. [1] Montoya-Pino et al. (2010) Geology, 38, 315-318 [2] Romaniello et al. (2013) 362, 305-316 [3] Andersen et al. (2014) EPSL, 400, 184-194 [4] Westermann et al. (2010) Cret. Res., 31, 500-514

Influence of glacial meltwater on global seawater δ234U

NASA Astrophysics Data System (ADS)

Arendt, Carli A.; Aciego, Sarah M.; Sims, Kenneth W. W.; Das, Sarah B.; Sheik, Cody; Stevenson, Emily I.

2018-03-01

We present the first published uranium-series measurements from modern Greenland Ice Sheet (GrIS) runoff and proximal seawater, and investigate the influence of glacial melt on global seawater δ234U over glacial-interglacial (g-ig) timescales. Climate reconstructions based on closed-system uranium-thorium (U/Th) dating of fossil corals assume U chemistry of seawater has remained stable over time despite notable fluctuations in major elemental compositions, concentrations, and isotopic compositions of global seawater on g-ig timescales. Deglacial processes increase weathering, significantly increasing U-series concentrations and changing the δ234U of glacial meltwater. Analyses of glacial discharge from GrIS outlet glaciers indicate that meltwater runoff has elevated U concentrations and differing 222Rn concentrations and δ234U compositions, likely due to variations in subglacial residence time. Locations with high δ234U have the potential to increase proximal seawater δ234U. To better understand the impact of bulk glacial melt on global seawater δ234U over time, we use a simple box model to scale these processes to periods of extreme deglaciation. We account for U fluxes from the GrIS, Antarctica, and large Northern Hemisphere Continental Ice Sheets, and assess sensitivity by varying melt volumes, duration and U flux input rates based on modern subglacial water U concentrations and compositions. All scenarios support the hypothesis that global seawater δ234U has varied by more than 1‰ through time as a function of predictable perturbations in continental U fluxes during g-ig periods.

Evaluating Uranium Isotopes in Carbonates and Implications for Reconstructing Marine Paleoredox Conditions

NASA Astrophysics Data System (ADS)

Aharony, Ofer; Gubser, Steven S.; Maldacena, Juan; Ooguri, Hirosi; Oz, Yaron

2016-12-01

Uranium isotope ratios (238U/235U, reported as δ238U) have emerged as a promising proxy for marine redox conditions. This proxy relies on isotopic fractionation that occurs during reduction of soluble U(VI) to insoluble U(IV), wherein 238U is preferentially reduced and incorporated via authigenic processes into anoxic sediments, leaving the residual seawater U and resulting carbonates 238U-depleted. Because carbonates are generally well preserved in the rock record, they are useful archives of seawater chemistry throughout Earth history, including δ238U. In principle, the long residence time of U in the ocean permits quantitative inferences of global paleoredox conditions using carbonate δ238U records. To assess the performance of the proxy, we compile all published δ238U measurements from carbonate rocks and sediments, which span the Cryogenian through the modern. The potential for δ238U to serve as a quantitative, global paleoredox proxy is supported by reproducible trends across depositional environments and paleogeographic regions in the Cryogenian non-glacial interlude and across the Permian-Triassic and Triassic-Jurassic boundaries, although carbonates deposited in deeper waters (>200 m) may be subject to local effects. Using a box model, we highlight the key levers associated with seawater δ238U and the timescales of such variability. Like all sedimentary archives, carbonate rocks are prone to diagenetic alteration and additional controls that cause δ238U in carbonates to deviate from global seawater values. Specifically, the U isotopic composition of carbonate sediments can be influenced by diagenesis, carbonate mineralogy, dolomitization, detrital input, local organic matter deposition, and pore water chemistry. We evaluate indicators of these factors in the context of a diagenetic model to assess the sensitivity of carbonate δ238U to local syndepositional or post-depositional processes. These results improve the framework for interpreting carbonate δ238U records and reconstructing past changes in the oxygenation of the Earth's oceans.

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.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ullmann, J. L.; Kawano, T.; Baramsai, B.

The cross section for neutron capture in the continuum region has been difficult to calculate accurately. Previous results for 238 U show that including an M 1 scissors-mode contribution to the photon strength function resulted in very good agreement between calculation and measurement. Our paper extends that analysis to 234 , 236 U by using γ -ray spectra measured with the Detector for Advanced Neutron Capture Experiments (DANCE) at the Los Alamos Neutron Science Center to constrain the photon strength function used to calculate the capture cross section. Calculations using a strong scissors-mode contribution reproduced the measured γ -ray spectramore » and were in excellent agreement with the reported cross sections for all three isotopes.« less

238U/235U determinations of some commonly used reference materials and U-bearing accessory minerals (Invited)

NASA Astrophysics Data System (ADS)

Condon, D.; Noble, S.; McLean, N.; Bowring, S. A.

2009-12-01

We have determined 238U/235U ratios for a suite of commonly used natural (CRM 112a, SRM 950a, HU-1) and synthetic (IRMM 184 and CRM U500) uranium reference materials in addition to several U-bearing accessory phases (zircon and monazite) by thermal ionisation mass-spectrometry (TIMS) using the IRMM 3636 233U-236U double spike to accurately correct for mass fractionation. The 238U/235U values for the natural uranium reference materials differ, by up to 0.1%, from the widely used ‘consensus’ value (137.88) with all having 238U/235U values less than 137.88. Similarly, initial 238U/235U data from zircon and monazite yield 238U/235U values that are lower than the ‘consensus’ value. The data obtained from U-bearing minerals is used to assess how the uncertainty in the 238U/235U ratio contributes to the systematic discordance observed in 238U/206Pb and 235U/207Pb dates (Mattinson, 2000; Schoene et al., 2006) which has traditionally been wholly attributed to error in the U decay constants. The 238U/235U determinations made on the synthetic reference materials yield results that are considerably more precise and accurate than the certified values (0.02% vs. 0.1% for CRM U500). The calibration of isotopic tracers used for U-daughter geochronology that are partially based upon these reference materials, and the resultant age determinations, will benefit from increased accuracy and precision. Mattinson, J.M., 2000. Revising the “gold standard”—the uranium decay constants of Jaffey et al., 1971. Eos Trans. AGU, Spring Meet. Suppl., Abstract V61A-02. Schoene B., Crowley J.L., Condon D.C., Schmitz M.D., Bowring S.A., 2006, Reassessing the uranium decay constants for geochronology using ID-TIMS U-Pb data. Geochimica et Cosmochimica Acta 70: 426-445

Uranium and its decay products in samples contaminated with uranium mine and mill waste

NASA Astrophysics Data System (ADS)

Benedik, L.; Klemencic, H.; Repinc, U.; Vrecek, P.

2003-05-01

The routine determination of the activity concentrations of uranium isotopes (^{238}U, ^{235}U and ^{234}U), thorium isotopes (^{212}Th, ^{230}TI, and ^{228}Th), ^{231}Pa, ^{226}Ra, ^{210}Pb and ^{210}Po in the environment is one of the most important tasks in uranium mining areas. Natural radionuclides contribute negligibly to the extemal radiation dose, but in the case of ingestion or inhalation can represent a very serious hazard. The objective of this study was to determine the activities of uranium and its decay products ^{230}Th, ^{231}Pa, ^{226}Ra, ^{210}Pb and ^{210}Po in sediments and water below sources of contamination (uranium mine, disposal sites and individual inflows) using gamma and alpha spectrometry, beta counting, the liquid scintillation technique and radiochemical neutron activation analysis.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

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.more » 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.« less

Uranium in mining water of kaolin open pit in Zarów (Lower Silesia); methodology of determination and genetic remarks.

PubMed

Chau, N D; Wyszomirski, P; Chruściel, E; Ochoński, A

1999-11-01

In this paper, a method of determination of uranium 238 and 234 in mining waters of Andrzej kaolin open pit in Zarów (Lower Silesia) is presented. The method is based on independent measurements of alpha and beta radiation intensities by means of a liquid scintillation spectrometer alpha/beta. The initial volume of water sample was 3 dm3, then it was diminished by chemical preparation to 6 cm3, and then 12 cm3 of scintillator was added. The lower limit of detection (for the measurement time of 8 h) for both 234U and 238U amounted to 0.02 Bq/dm3. For determination of the uranium content in ferruginous sediments precipitating from mining waters of the above-mentioned open pit, gamma ray spectrometry was used. The obtained results may be viewed as a contribution to studies on anomalous uranium concentration within this kaolin deposit. The elevated uranium content, in comparison with its average concentration in the Earth crust, is characteristic for parent rocks of Andrzej kaolin deposit, which are granitoids of Strzegom-Sobótka massif. In connection with it, the high uranium content can be observed not only in kaolin and weakly kaolinised granitoids from the deposit in question, but also in mining waters genetically related with them.

Trace metal cycling and 238U/235U in New Zealand's fjords: Implications for reconstructing global paleoredox conditions in organic-rich sediments

NASA Astrophysics Data System (ADS)

Hinojosa, Jessica L.; Stirling, Claudine H.; Reid, Malcolm R.; Moy, Christopher M.; Wilson, Gary S.

2016-04-01

Reconstructing the history of ocean oxygenation provides insight into links between ocean anoxia, biogeochemical cycles, and climate. Certain redox-sensitive elements respond to changes in marine oxygen content through phase shifts and concomitant isotopic fractionation, providing new diagnostic proxies of past ocean hypoxia. Here we explore the behavior and inter-dependence of a suite of commonly utilized redox-sensitive trace metals (U, Mo, Fe, and Mn) and the emerging ;stable; isotope system of U (238U/235U, or δ238U) in New Zealand fjords. These semi-restricted basins have chemical conditions spanning the complete redox spectrum from fully oxygenated to suboxic to intermittently anoxic/euxinic. In the anoxic water column, U and Mo concentrations decrease, while Fe and Mn concentrations increase. Similarly, signals of past euxinic conditions can be found by U, Mo, Fe, and Mn enrichment in the underlying sediments. The expected U isotopic shift toward a lower δ238U in the anoxic water column due to U(VI)-U(IV) reduction is not observed; instead, water column δ238U profiles are consistent in fjords of all oxygen content, falling within previously reported ranges for open ocean seawater (δ238U = -0.42 ± 0.07‰). Additionally, surface sediment δ238U results show evidence for competing U isotope fractionation processes. One site indicates increased export of 238U from seawater to the underlying sediments (fractionation between aqueous seawater U and particulate sediment U, or ΔU(aq)-U(solid) = -0.25‰), consistent with redox-driven fractionation. Another site suggests potential U(VI) adsorption-driven fractionation, reflecting increased export of 235U from seawater to sediments (ΔU(aq)-U(solid) = 0.25‰). We discuss several potential factors that could alter δ238U in waters and sediments beyond redox-driven shifts, including adsorption to organic matter in waters of high primary productivity, reaction rates for competing processes of U adsorption and release, and isotopic constraints of U coming into the system from terrestrial environments. These potential complications should be understood and constrained through observations, experiments, and models before future application of δ238U as a global paleoredox tracer can achieve its full potential.

Distribution of U-Th nuclides in the riverine and coastal environments of the tropical southwest coast of India.

PubMed

Balakrishna, K; Shankar, R; Sarin, M M; Manjunatha, B R

2001-01-01

A reconnaissance study has been made on the distribution of 238U, 234U, 232Th and 230Th in soils, water, suspended particulate matter (SPM) and bottom sediments in the Kali river basin around Kaiga, its estuarine region and the adjacent Arabian Sea to obtain the baseline data of U-Th series nuclides in view of the commissioning of nuclear power reactors at Kaiga, near Karwar, on the southwest coast of India. Drainage basin soils developed over greywackes (the dominant litho-unit upstream) are lower in 238U/Al and 232Th/Al ratios by factors of 3-5 in comparison with those developed over tonalitic gneisses (the dominant litho-unit downstream). The dominance of the former type of soils is reflected in the composition of river-bottom sediments derived from the upstream drainage basin during the monsoon. The 232Th in bottom sediments tends to increase towards the estuarine and coastal areas, presumably due to deposition of heavy minerals and onshore transport of coastal sediments into the estuary. The dissolved U in the Kali river is low (0.001-0.02 microg/l) when compared to the major Indian rivers as the Kali river flows through U-poor greywackes. Thus, the input of dissolved U to the Kali estuary is dominated by sea water. Although there is some evidence for the removal of dissolved U at low salinity during estuarine mixing, its behaviour is conservative in the lower estuary (at higher salinities). The removal rate of dissolved U from the Kali river basin is similar to that reported from other tropical river basins. The U flux from all the west-flowing rivers of Peninsular India is estimated at 26.3 x 10(6) g/yr to the Arabian Sea which is about 2% of the flux from the Himalayan rivers to the Bay of Bengal.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kayzar, Theresa M.; Villa, Adam C.; Lobaugh, Megan L.

The uranium concentrations and isotopic compositions of waters, sediment leachates and sediments from Red Rock Creek in the Stanislaus National Forest of California were measured to investigate the transport of uranium from a point source (the Juniper Uranium Mine) to a natural surface stream environment. Furthermore, we alter the (234U)/(238U) composition of Red Rock Creek downstream of the Juniper Mine. As a result of mine-derived contamination, water (234U)/(238U) ratios are 67% lower than in water upstream of the mine (1.114–1.127 ± 0.009 in the contaminated waters versus 1.676 in the clean branch of the stream), and sediment samples have activitymore » ratios in equilibrium in the clean creek and out of equilibrium in the contaminated creek (1.041–1.102 ± 0.007). Uranium concentrations in water, sediment and sediment leachates are highest downstream of the mine, but decrease rapidly after mixing with the clean branch of the stream. Uranium content and compositions of the contaminated creek headwaters relative to the mine tailings of the Juniper Mine suggest that uranium has been weathered from the mine and deposited in the creek. The distribution of uranium between sediment surfaces (leachable fraction) and bulk sediment suggests that adsorption is a key element of transfer along the creek. In clean creek samples, uranium is concentrated in the sediment residues, whereas in the contaminated creek, uranium is concentrated on the sediment surfaces (~70–80% of uranium in leachable fraction). Furthermore, contamination only exceeds the EPA maximum contaminant level (MCL) for drinking water in the sample with the closest proximity to the mine. Isotopic characterization of the uranium in this system coupled with concentration measurements suggest that the current state of contamination in Red Rock Creek is best described by mixing between the clean creek and contaminated upper branch of Red Rock Creek rather than mixing directly with mine sediment.« less

Radioactivity contents in dicalcium phosphate and the potential radiological risk to human populations.

PubMed

Casacuberta, N; Masqué, P; Garcia-Orellana, J; Bruach, J M; Anguita, M; Gasa, J; Villa, M; Hurtado, S; Garcia-Tenorio, R

2009-10-30

Potentially harmful phosphate-based products derived from the wet acid digestion of phosphate rock represent one of the most serious problems facing the phosphate industry. This is particularly true for dicalcium phosphate (DCP), a food additive produced from either sulphuric acid or hydrochloric acid digestion of raw rock material. This study determined the natural occurring radionuclide concentrations of 12 DCP samples and 4 tricalcium phosphate (TCP) samples used for animal and human consumption, respectively. Metal concentrations (Al, Fe, Zn, Cd, Cr, As, Hg, Pb and Mg) were also determined. Samples were grouped into three different clusters (A, B, C) based on their radionuclide content. Whereas group A is characterized by high activities of 238U, 234U (approximately 10(3) Bq kg(-1)), 210Pb (2 x 10(3) Bq kg(-1)) and (210)Po ( approximately 800 Bq kg(-1)); group B presents high activities of (238)U, (234)U and (230)Th (approximately 10(3) Bq kg(-1)). Group C was characterized by very low activities of all radionuclides (< 50 Bq kg(-1)). Differences between the two groups of DCP samples for animal consumption (groups A and B) were related to the wet acid digestion method used, with group A samples produced from hydrochloric acid digestion, and group B samples produced using sulphuric acid. Group C includes more purified samples required for human consumption. High radionuclide concentrations in some DCP samples (reaching 2 x 10(3) and 10(3) Bq kg(-1) of 210Pb and 210Po, respectively) may be of concern due to direct or indirect radiological exposure via ingestion. Our experimental results based on 210Pb and 210Po within poultry consumed by humans, suggest that the maximum radiological doses are 11 +/- 2 microSv y(-1). While these results suggest that human health risks are small, additional testing should be conducted.

Sediment transport time measured with U-Series isotopes: Resultsfrom ODP North Atlantic Drill Site 984

DOE Office of Scientific and Technical Information (OSTI.GOV)

DePaolo, Donald J.; Maher, Kate; Christensen, John N.

High precision uranium isotope measurements of marineclastic sediments are used to measure the transport and storage time ofsediment from source to site of deposition. The approach is demonstratedon fine-grained, late Pleistocene deep-sea sediments from Ocean DrillingProgram Site 984A on the Bjorn Drift in the North Atlantic. The sedimentsare siliciclastic with up to 30 percent carbonate, and dated by sigma 18Oof benthic foraminifera. Nd and Sr isotopes indicate that provenance hasoscillated between a proximal source during the last three interglacialperiods volcanic rocks from Iceland and a distal continental sourceduring glacial periods. An unexpected finding is that the 234U/238Uratios of the silicatemore » portion of the sediment, isolated by leaching withhydrochloric acid, are significantly less than the secular equilibriumvalue and show large and systematic variations that are correlated withglacial cycles and sediment provenance. The 234U depletions are inferredto be due to alpha-recoil loss of234Th, and are used to calculate"comminution ages" of the sediment -- the time elapsed between thegeneration of the small (<_ 50 mu-m) sediment grains in the sourceareas by comminution of bedrock, and the time of deposition on theseafloor. Transport times, the difference between comminution ages anddepositional ages, vary from less than 10 ky to about 300 to 400 ky forthe Site 984A sediments. Long transport times may reflect prior storagein soils, on continental shelves, or elsewhere on the seafloor. Transporttime may also be a measure of bottom current strength. During the mostrecent interglacial periods the detritus from distal continental sourcesis diluted with sediment from Iceland that is rapidly transported to thesite of deposition. The comminution age approach could be used to dateQuaternary non-marine sediments, soils, and atmospheric dust, and may beenhanced by concomitant measurement of 226Ra/230Th, 230Th/234U, andcosmogenic nuclides.« less

U(v) in metal uranates: A combined experimental and theoretical study of MgUO 4, CrUO 4, and FeUO 4

DOE PAGES

Guo, Xiaofeng; Tiferet, Eitan; Qi, Liang; ...

2016-01-01

Although pentavalent uranium can exist in aqueous solution, its presence in the solid state is uncommon. Metal monouranates, MgUO 4, CrUO 4 and FeUO 4 were synthesized for detailed structural and energetic investigations. Structural characteristics of these uranates used powder X-ray diffraction, synchrotron X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe-Mossbauer spectroscopy. Enthalpies of formation were measured by high temperature oxide melt solution calorimetry. Density functional theory (DFT) calculations provided both structural and energetic information. The measured structural and thermodynamic properties show good consistency with those predicted from DFT. The presence of U 5+ has been solidly confirmed in CrUOmore » 4 and FeUO 4, which are thermodynamically stable compounds, and the origin and stability of U 5+ in the system was elaborated by DFT. Lastly, the structural and thermodynamic behaviour of U 5+ elucidated in this work is relevant to fundamental actinide redox chemistry and to applications in the nuclear industry and radioactive waste disposal.« less

The study of equivalent dose of uranium in long bean (V. U. Sesquipedalis) and the effect on human

NASA Astrophysics Data System (ADS)

Rashid, Nur Shahidah Abdul; Yoshandi, Tengku Mohammad; Majid, Sukiman Sarmania Amran Ab.; Mohamed, Faizal; Siong, Khoo Kok

2016-01-01

In the case of accidental release of Uranium-238 (238U) radionuclides in a nuclear facility or in the environment, internal contamination by either acute or chronic exposure has the potential to induce both radiological and chemical toxic effects. A study was conducted to estimate the 238U radionuclide concentration in the long beans using Induced Coupled Mass Plasma-Spectrometry (ICP-MS). 238U radionuclide is a naturally occurring radioactive material that can be found in soil and can be transferred to the long bean (Vigna unguiculata subsp. Sesquapedalis) directly or indirectly via water or air. Kidney and liver are the major sites of deposition of 238U radionuclide. The obtained dose exposed in the liver and kidney is used to assess the safety level for public intake of 238U radionuclide from the consumption of long beans. The concentration of 238U radionuclide measured in long bean samples was 0.0226 ± 0.0009 mg/kg. Total activity of 238U radionuclide was 0.0044 ± 0.0002 Bq/day with the daily intake of 0.3545 ± 0.0143 µg/day and the annual committed effective dose due to ingestion of 238U radionuclide in long beans was 0.2230 ± 0.0087 µSv/year. The committed equivalent dose of 238U radionuclide from the assessment in the liver and kidney are 0.4198 ± 0.0165 nSv and 10.9335 ± 0.4288 nSv. The risk of cancer of 238U radionuclide was determined to be (86.0466 ± 3.3748) × 10-9. Thus, the results concluded that 238U radionuclide in local long beans was in the permitted level and safe to consume without posing any significant radiological threat to population.

Short-lived U and Th isotope distribution in a tropical laterite derived from granite (Pitinga river basin, Amazonia, Brazil): Application to assessment of weathering rate

NASA Astrophysics Data System (ADS)

Mathieu, D.; Bernat, M.; Nahon, D.

1995-12-01

We have analyzed samples of a 15 m thick profile weathered from the Madeira granite, located in the Pitinga basin river, north of Manaus, in the state of Amazonia, Brazil. This profile consists essentially of a yellow-red saprolite covered by a soil. U and Th concentrations are particularly high in the granite (20 and 80 μg/g respectively). Normalized element to Th concentrations indicate that Th is most resistant to chemical weathering, except to some extent in the top soil. Higher concentrations in the saprolite compared to the granite comprise a relative enrichment, resulting from a loss of mass. The saprolites are initially generated by a descending weathering front which alters the granite to a yellow-red saprolite, a second front, close to the top, turns the saprolite into a soil. Weathering has led to leaching of U. The 234U/ 238U and 230Th/ 238U isotopic ratios are in radioactive disequilibrium. Numerous nodules are present and apparently started to form at the base of the saprolite. These nodules achieve more developed form during their relative ascent until they are reached by the descending top front where they undergo dissolution. The Th and Pb are concentrated in the nodules close to the top front. The U, being more mobile, is strongly leached by the first front, and most of the remainder, freed by the second, engages in a descending flux which supplies the underlying saprolite. Using the data an attempt is made to model the isotopic distribution in the profile. We conclude that the first front has descended at a rate of 5 cm/1000 yt, and that the time needed to create the saprolite must have been around 300,000 yr.

Characterization of cores from an in-situ recovery mined uranium deposit in Wyoming: Implications for post-mining restoration

DOE Office of Scientific and Technical Information (OSTI.GOV)

WoldeGabriel, G.; Boukhalfa, H.; Ware, S. D.

In-situ recovery (ISR) of uranium (U) from sandstone-type roll-front deposits is a technology that involves the injection of solutions that consist of ground water fortified with oxygen and carbonate to promote the oxidative dissolution of U, which is pumped to recovery facilities located at the surface that capture the dissolved U and recycle the treated water. The ISR process alters the geochemical conditions in the subsurface creating conditions that are more favorable to the migration of uranium and other metals associated with the uranium deposit. There is a lack of clear understanding of the impact of ISR mining on themore » aquifer and host rocks of the post-mined site and the fate of residual U and other metals within the mined ore zone. We performed detailed petrographic, mineralogical, and geochemical analyses of several samples taken from about 7 m of core of the formerly the ISR-mined Smith Ranch–Highland uranium deposit in Wyoming. We show that previously mined cores contain significant residual uranium (U) present as coatings on pyrite and carbonaceous fragments. Coffinite was identified in three samples. Core samples with higher organic (> 1 wt.%) and clay (> 6–17 wt.%) contents yielded higher 234U/ 238U activity ratios (1.0–1.48) than those with lower organic and clay fractions. The ISR mining was inefficient in mobilizing U from the carbonaceous materials, which retained considerable U concentrations (374–11,534 ppm). This is in contrast with the deeper part of the ore zone, which was highly depleted in U and had very low 234U/ 238U activity ratios. This probably is due to greater contact with the lixiviant (leaching solution) during ISR mining. EXAFS analyses performed on grains with the highest U and Fe concentrations reveal that Fe is present in a reduced form as pyrite and U occurs mostly as U(IV) complexed by organic matter or as U(IV) phases of carbonate complexes. Moreover, U–O distances of ~ 2.05 Å were noted, indicating the potential formation of other poorly defined U(IV/VI) species. We also noted a small contribution from Udouble bond; length as m-dashO at 1.79 Å, which indicates that U is partially oxidized. There is no apparent U–S or U–Fe interaction in any of the U spectra analyzed. However, SEM analysis of thin sections prepared from the same core material reveals surficial U associated with pyrite which is probably a minor fraction of the total U present as thin coatings on the surface of pyrite. Our data show the presence of different structurally variable uranium forms associated with the mined cores. U associated with carbonaceous materials is probably from the original U mobilization that accumulated in the organic matter-rich areas under reducing conditions during shallow burial diagenesis. U associated with pyrite represents a small fraction of the total U and was likely deposited as a result of chemical reduction by pyrite. Our data suggest that areas rich in carbonaceous materials had limited exposure to the lixiviant solution, continue to be reducing, and still hold significant U resources. Because of their limited access to fluid flow, these areas might not contribute significantly to post-mining U release or attenuation. Areas with pyrite that are accessible to fluids seem to be more reactive and could act as reductants and facilitate U reduction and accumulation, limiting its migration.« less

Characterization of cores from an in-situ recovery mined uranium deposit in Wyoming: Implications for post-mining restoration

DOE PAGES

WoldeGabriel, G.; Boukhalfa, H.; Ware, S. D.; ...

2014-10-08

In-situ recovery (ISR) of uranium (U) from sandstone-type roll-front deposits is a technology that involves the injection of solutions that consist of ground water fortified with oxygen and carbonate to promote the oxidative dissolution of U, which is pumped to recovery facilities located at the surface that capture the dissolved U and recycle the treated water. The ISR process alters the geochemical conditions in the subsurface creating conditions that are more favorable to the migration of uranium and other metals associated with the uranium deposit. There is a lack of clear understanding of the impact of ISR mining on themore » aquifer and host rocks of the post-mined site and the fate of residual U and other metals within the mined ore zone. We performed detailed petrographic, mineralogical, and geochemical analyses of several samples taken from about 7 m of core of the formerly the ISR-mined Smith Ranch–Highland uranium deposit in Wyoming. We show that previously mined cores contain significant residual uranium (U) present as coatings on pyrite and carbonaceous fragments. Coffinite was identified in three samples. Core samples with higher organic (> 1 wt.%) and clay (> 6–17 wt.%) contents yielded higher 234U/ 238U activity ratios (1.0–1.48) than those with lower organic and clay fractions. The ISR mining was inefficient in mobilizing U from the carbonaceous materials, which retained considerable U concentrations (374–11,534 ppm). This is in contrast with the deeper part of the ore zone, which was highly depleted in U and had very low 234U/ 238U activity ratios. This probably is due to greater contact with the lixiviant (leaching solution) during ISR mining. EXAFS analyses performed on grains with the highest U and Fe concentrations reveal that Fe is present in a reduced form as pyrite and U occurs mostly as U(IV) complexed by organic matter or as U(IV) phases of carbonate complexes. Moreover, U–O distances of ~ 2.05 Å were noted, indicating the potential formation of other poorly defined U(IV/VI) species. We also noted a small contribution from Udouble bond; length as m-dashO at 1.79 Å, which indicates that U is partially oxidized. There is no apparent U–S or U–Fe interaction in any of the U spectra analyzed. However, SEM analysis of thin sections prepared from the same core material reveals surficial U associated with pyrite which is probably a minor fraction of the total U present as thin coatings on the surface of pyrite. Our data show the presence of different structurally variable uranium forms associated with the mined cores. U associated with carbonaceous materials is probably from the original U mobilization that accumulated in the organic matter-rich areas under reducing conditions during shallow burial diagenesis. U associated with pyrite represents a small fraction of the total U and was likely deposited as a result of chemical reduction by pyrite. Our data suggest that areas rich in carbonaceous materials had limited exposure to the lixiviant solution, continue to be reducing, and still hold significant U resources. Because of their limited access to fluid flow, these areas might not contribute significantly to post-mining U release or attenuation. Areas with pyrite that are accessible to fluids seem to be more reactive and could act as reductants and facilitate U reduction and accumulation, limiting its migration.« less

Investigating Pu and U isotopic compositions in sediments: a case study in Lake Obuchi, Rokkasho Village, Japan using sector-field ICP-MS and ICP-QMS.

PubMed

Zheng, Jian; Yamada, Masatoshi

2005-08-01

The objectives of the present work were to study isotope ratios and the inventory of plutonium and uranium isotope compositions in sediments from Lake Obuchi, which is in the vicinity of several nuclear fuel facilities in Rokkasho, Japan. Pu and its isotopes were determined using sector-field ICP-MS and U and its isotopes were determined with ICP-QMS after separation and purification with a combination of ion-exchange and extraction chromatography. The observed (240)Pu/(239)Pu atom ratio (0.186 +/- 0.016) was similar to that of global fallout, indicating that the possible early tropospheric fallout Pu did not deliver Pu from the Pacific Proving Ground to areas above 40 degrees N. The previously reported higher Pu inventory in the deep water area of Lake Obuchi could be attributed to the lateral transportation of Pu deposited in the shallow area which resulted from the migration of deposited global fallout Pu from the land into the lake by river runoff and from the Pacific Ocean by tide movement and sea water scavenging, as well as from direct soil input by winds. The (235)U/(238)U atom ratios ranged from 0.00723 to 0.00732, indicating the natural origin of U in the sediments. The average (234)U/(238)U activity ratio of 1.11 in a sediment core indicated a significant sea water U contribution. No evidence was found for the release of U containing wastes from the nearby nuclear facilities. These results will serve as a reference baseline on the levels of Pu and U in the studied site so that any further contamination from the spent nuclear fuel reprocessing plants, the radioactive waste disposal and storage facilities, and the uranium enrichment plant can be identified, and the impact of future release can be rapidly assessed.

Testing models of thorium and particle cycling in the ocean using data from station GT11-22 of the U.S. GEOTRACES North Atlantic section

NASA Astrophysics Data System (ADS)

Lerner, Paul; Marchal, Olivier; Lam, Phoebe J.; Anderson, Robert F.; Buesseler, Ken; Charette, Matthew A.; Edwards, R. Lawrence; Hayes, Christopher T.; Huang, Kuo-Fang; Lu, Yanbin; Robinson, Laura F.; Solow, Andrew

2016-07-01

Thorium is a highly particle-reactive element that possesses different measurable radio-isotopes in seawater, with well-constrained production rates and very distinct half-lives. As a result, Th has emerged as a key tracer for the cycling of marine particles and of their chemical constituents, including particulate organic carbon. Here two different versions of a model of Th and particle cycling in the ocean are tested using an unprecedented data set from station GT11-22 of the U.S. GEOTRACES North Atlantic Section: (i) 228,230,234Th activities of dissolved and particulate fractions, (ii) 228Ra activities, (iii) 234,238U activities estimated from salinity data and an assumed 234U/238U ratio, and (iv) particle concentrations, below a depth of 125 m. The two model versions assume a single class of particles but rely on different assumptions about the rate parameters for sorption reactions and particle processes: a first version (V1) assumes vertically uniform parameters (a popular description), whereas the second (V2) does not. Both versions are tested by fitting to the GT11-22 data using generalized nonlinear least squares and by analyzing residuals normalized to the data errors. We find that model V2 displays a significantly better fit to the data than model V1. Thus, the mere allowance of vertical variations in the rate parameters can lead to a significantly better fit to the data, without the need to modify the structure or add any new processes to the model. To understand how the better fit is achieved we consider two parameters, K =k1 /(k-1 +β-1) and K/P, where k1 is the adsorption rate constant, k-1 the desorption rate constant, β-1 the remineralization rate constant, and P the particle concentration. We find that the rate constant ratio K is large (⩾ 0.2) in the upper 1000 m and decreases to a nearly uniform value of ca. 0.12 below 2000 m, implying that the specific rate at which Th attaches to particles relative to that at which it is released from particles is higher in the upper ocean than in the deep ocean. In contrast, K/P increases with depth below 500 m. The parameters K and K/P display significant positive and negative monotonic relationship with P, respectively, which is collectively consistent with a particle concentration effect.

Neutron capture cross-section measurements for 238U between 0.4 and 1.4 MeV

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Finch, S. W.; Howell, C. R.; Tonchev, A. P.; Tornow, W.

2017-09-01

Neutron-induced radiative-capture cross-section data of 238U are crucial for fundamental nuclear physics as well as for Stewardship Science, for advanced-fuel-cycle calculations, and for nuclear astrophysics. Based on different techniques, there are a large number of 238U(n, γ) 239U cross-section data available in the literature. However, there is a lack of systematic and consistent measurements in the 0.1 to 3.0 MeV energy range. The goal of the neutron-capture project at TUNL is to provide accurate 238U(n, γ) 239U cross-section data in this energy range. The 238U samples, sandwiched between gold foils of the same size, were irradiated for 8-14 hours with monoenergetic neutrons. To avoid any contribution from thermal neutrons, the 238U and 197Au targets were placed inside of a thin-walled pill-box made of 238U. Finally, the whole pill-box was wrapped in a gold foil as well. After irradiation, the samples were gamma-counted at the TUNL's low-background counting facility using high-efficient HPGe detectors. The 197Au monitor foils were used to calculate the neutron flux. The experimental technique and 238U(n, γ) 239U cross-section results at 6 energies will be discussed during the meeting.

230Th/U ages Supporting Hanford Site-Wide Probabilistic Seismic Hazard Analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paces, James B.

This product represents a USGS Administrative Report that discusses samples and methods used to conduct uranium-series isotope analyses and resulting ages and initial 234U/238U activity ratios of pedogenic cements developed in several different surfaces in the Hanford area middle to late Pleistocene. Samples were collected and dated to provide calibration of soil development in surface deposits that are being used in the Hanford Site-Wide probabilistic seismic hazard analysis conducted by AMEC. The report includes description of sample locations and physical characteristics, sample preparation, chemical processing and mass spectrometry, analytical results, and calculated ages for individual sites. Ages of innermost rindsmore » on a number of samples from five sites in eastern Washington are consistent with a range of minimum depositional ages from 17 ka for cataclysmic flood deposits to greater than 500 ka for alluvium at several sites.« less

230Th/U ages Supporting Hanford Site‐Wide Probabilistic Seismic Hazard Analysis

USGS Publications Warehouse

Paces, James B.

2014-01-01

This product represents a USGS Administrative Report that discusses samples and methods used to conduct uranium-series isotope analyses and resulting ages and initial 234U/238U activity ratios of pedogenic cements developed in several different surfaces in the Hanford area middle to late Pleistocene. Samples were collected and dated to provide calibration of soil development in surface deposits that are being used in the Hanford Site-Wide probabilistic seismic hazard analysis conducted by AMEC. The report includes description of sample locations and physical characteristics, sample preparation, chemical processing and mass spectrometry, analytical results, and calculated ages for individual sites. Ages of innermost rinds on a number of samples from five sites in eastern Washington are consistent with a range of minimum depositional ages from 17 ka for cataclysmic flood deposits to greater than 500 ka for alluvium at several sites.

Evaluation of the suitability of neural network method for prediction of uranium activity ratio in environmental alpha spectra.

PubMed

Einian, Mohammad Reza; Aghamiri, Seyed Mahmood Reza; Ghaderi, Reza

2015-11-01

Applying Artificial Neural Network to an alpha spectrometry system is a good idea to discriminate the composition of environmental and non-environmental materials by the estimation of the (234)U/(238)U activity ratio. Because it eliminates limitations of classical approaches by the extraction the desired information from the average of a partial uranium raw spectrum. The network was trained by an alpha spectrum library which was developed in this work. The results indicated that there was a small difference between the target values and the predictions. These results were acceptable, because the thickness of samples and the inferring elements were different in the real library. Copyright © 2015 Elsevier Ltd. All rights reserved.

Application of the 226Ra– 230Th– 234U and 227Ac– 231Pa– 235U radiochronometers to uranium certified reference materials

DOE PAGES

Rolison, John M.; Treinen, Kerri C.; McHugh, Kelly C.; ...

2017-11-06

Uranium certified reference materials (CRM) issued by New Brunswick Laboratory were subjected to dating using four independent uranium-series radiochronometers. In all cases, there was acceptable agreement between the model ages calculated using the 231Pa– 235U, 230Th– 234U, 227Ac– 235U or 226Ra– 234U radiochronometers and either the certified 230Th– 234U model date (CRM 125-A and CRM U630), or the known purification date (CRM U050 and CRM U100). Finally, the agreement between the four independent radiochronometers establishes these uranium certified reference materials as ideal informal standards for validating dating techniques utilized in nuclear forensic investigations in the absence of standards with certifiedmore » model ages for multiple radiochronometers.« less

Application of the 226Ra– 230Th– 234U and 227Ac– 231Pa– 235U radiochronometers to uranium certified reference materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rolison, John M.; Treinen, Kerri C.; McHugh, Kelly C.

Uranium certified reference materials (CRM) issued by New Brunswick Laboratory were subjected to dating using four independent uranium-series radiochronometers. In all cases, there was acceptable agreement between the model ages calculated using the 231Pa– 235U, 230Th– 234U, 227Ac– 235U or 226Ra– 234U radiochronometers and either the certified 230Th– 234U model date (CRM 125-A and CRM U630), or the known purification date (CRM U050 and CRM U100). Finally, the agreement between the four independent radiochronometers establishes these uranium certified reference materials as ideal informal standards for validating dating techniques utilized in nuclear forensic investigations in the absence of standards with certifiedmore » model ages for multiple radiochronometers.« less

The study of equivalent dose of uranium in long bean (V. U. Sesquipedalis) and the effect on human

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rashid, Nur Shahidah Abdul; Yoshandi, Tengku Mohammad; Majid, Sukiman Sarmania Amran Ab.

In the case of accidental release of Uranium-238 ({sup 238}U) radionuclides in a nuclear facility or in the environment, internal contamination by either acute or chronic exposure has the potential to induce both radiological and chemical toxic effects. A study was conducted to estimate the {sup 238}U radionuclide concentration in the long beans using Induced Coupled Mass Plasma-Spectrometry (ICP-MS). {sup 238}U radionuclide is a naturally occurring radioactive material that can be found in soil and can be transferred to the long bean (Vigna unguiculata subsp. Sesquapedalis) directly or indirectly via water or air. Kidney and liver are the major sitesmore » of deposition of {sup 238}U radionuclide. The obtained dose exposed in the liver and kidney is used to assess the safety level for public intake of {sup 238}U radionuclide from the consumption of long beans. The concentration of {sup 238}U radionuclide measured in long bean samples was 0.0226 ± 0.0009 mg/kg. Total activity of {sup 238}U radionuclide was 0.0044 ± 0.0002 Bq/day with the daily intake of 0.3545 ± 0.0143 µg/day and the annual committed effective dose due to ingestion of {sup 238}U radionuclide in long beans was 0.2230 ± 0.0087 µSv/year. The committed equivalent dose of {sup 238}U radionuclide from the assessment in the liver and kidney are 0.4198 ± 0.0165 nSv and 10.9335 ± 0.4288 nSv. The risk of cancer of {sup 238}U radionuclide was determined to be (86.0466 ± 3.3748) × 10-9. Thus, the results concluded that {sup 238}U radionuclide in local long beans was in the permitted level and safe to consume without posing any significant radiological threat to population.« less

Geochronology and petrogenesis of MORB from the Juan de Fuca and Gorda ridges by 238U230Th disequilibrium

USGS Publications Warehouse

Goldstein, S.J.; Murrell, M.T.; Janecky, D.R.; Delaney, J.R.; Clague, D.A.

1991-01-01

A highly precise mass spectrometric method of analysis was used to determine 238U234U230Th232Th in axial and off-axis basalt glasses from Juan de Fuca (JDF) and Gorda ridges. Initial 230Th activity excesses in the axial samples range from 3 to 38%, but generally lie within a narrow range of 12 to 15%. Secondary alteration effects were evaluated using ??234U and appear to be negligible; hence the 230Th excesses are magmatic in origin. Direct dating of MORB was accomplished by measuring the decrease in excess 230Th in off-axis samples. 238U230Th ages progressively increase with distance from axis. Uncertainties in age range from 10 to 25 ka for UTh ages of 50 to 200 ka. The full spreading rate based on UTh ages for Endeavour segment of JDF is 5.9 ?? 1/2 cm/yr, with asymmetry in spreading between the Pacific (4.0 ?? 0.6 cm/yr) and JDF (1.9 ?? 0.6 cm/yr) plates. For northern Gorda ridge, the half spreading rate for the JDF plate is found to be 3.0 ?? 0.4 cm/yr. These rates are in agreement with paleomagnetic spreading rates and topographic constraints. This suggests that assumptions used to determine ages, including constancy of initial 230Th 232Th ratio over time, are generally valid for the areas studied. Samples located near the axis of spreading are typically younger than predicted by these spreading rates, which most likely reflects recent volcanism within a 1-3 km wide zone of crustal accretion. Initial 230Th/232Th ratios and 230Th activity were also used to examine the recent Th/U evolution and extent of melting of mantle sources beneath these ridges. A negative anomaly in 230Th 232Th for Axial seamount lavas provides the first geochemical evidence of a mantle plume source for Axial seamount and the Cobb-Eickelberg seamount chain and indicates recent depletion of other JDF segment sources. Large 230Th activity excesses for lavas from northern Gorda ridge and Endeavour segment indicate formation from a lower degree of partial melting than other segments. An inverse correlation between 230Th excess and 230Th 232Th for each ridge indicates that these lower degree melts formed from slightly less depleted sources than higher degree melts. Uniformity in 230Th excess for other segments suggests similarity in processes of melt formation and mixing beneath most of the JDF-Gorda ridge area. The average initial 230Th 232Th activity ratio of 1.31 for the JDF-Gorda ridge area is in agreement with the predicted value of 1.32 from the ThSr isotope mantle array. ?? 1991.

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.

Fission fragments mass distributions of nuclei populated by the multinucleon transfer channels of the 18O + 232Th reaction

NASA Astrophysics Data System (ADS)

Léguillon, R.; Nishio, K.; Hirose, K.; Makii, H.; Nishinaka, I.; Orlandi, R.; Tsukada, K.; Smallcombe, J.; Chiba, S.; Aritomo, Y.; Ohtsuki, T.; Tatsuzawa, R.; Takaki, N.; Tamura, N.; Goto, S.; Tsekhanovich, I.; Petrache, C. M.; Andreyev, A. N.

2016-10-01

It is shown that the multinucleon transfer reactions is a powerful tool to study fission of exotic neutron-rich actinide nuclei, which cannot be accessed by particle-capture or heavy-ion fusion reactions. In this work, multinucleon transfer channels of the 18O + 232Th reaction are used to study fission of fourteen nuclei 231,232,233,234Th, 232,233,234,235,236Pa, and 234,235,236,237,238U. Identification of fissioning nuclei and of their excitation energy is performed on an event-by-event basis, through the measurement of outgoing ejectile particle in coincidence with fission fragments. Fission fragment mass distributions are measured for each transfer channel, in selected bins of excitation energy. In particular, the mass distributions of 231,234Th and 234,235,236Pa are measured for the first time. Predominantly asymmetric fission is observed at low excitation energies for all studied cases, with a gradual increase of the symmetric mode towards higher excitation energy. The experimental distributions are found to be in general agreement with predictions of the fluctuation-dissipation model.

Heterogeneity in the 238U/235U Ratios of Angrites.

NASA Astrophysics Data System (ADS)

Tissot, F.; Dauphas, N.; Grove, T. L.

2016-12-01

Angrites are differentiated meteorites of basaltic composition, of either volcanic or plutonic origin, that display minimal post-crystallization alteration, metamorphism, shock or impact brecciation. Because quenched angrites cooled very rapidly, all radiochronometric systems closed simultaneously in these samples. Quenched angrites are thus often used as anchors for cross-calibrating short-lived dating methods (e.g., 26Al-26Mg) and the absolute dating techniques (e.g, Pb-Pb). Due to the constancy of the 238U/235U ratio in natural samples, Pb-Pb ages have long been calculated using a "consensus" 238U/235U ratio, but the discovery of resolvable variations in the 238U/235U ratio of natural samples, means that the U isotopic composition of the material to date also has to be determined in order to obtain high-precision Pb-Pb ages. We set out (a) to measure at high-precision the 238U/235U ratio of a large array of angrites to correct their Pb-Pb ages, and (b) to identify whether all angrites have a similar U isotopic composition, and, if not, what were the processes responsible for this variability. Recently, Brennecka & Wadhwa (2012) suggested that the angrite-parent body had a homogeneous 238U/235U ratio. They reached this conclusion partly because they propagated the uncertainties of the U isotopic composition of the various U double spikes that they used onto the final 238U/235U ratio the sample. Because this error is systematic (i.e., it affects all samples similarly), differences in the δ238U values of samples corrected by the same double spike are better known than one would be led to believe if uncertainties on the spike composition are propagated. At the conference, we will present the results of the high-precision U isotope analyses for six angrite samples: NWA 4590, NWA 4801, NWA 6291, Angra dos Reis, D'Orbigny, and Sahara 99555. We will show that there is some heterogeneity in the δ238U values of the angrites and will discuss the possible processes by which different angrite samples can acquire different U isotopic compositions. The U isotope data will then be used to correct Pb-Pb ages of angrites estimated using an assumed 238U/235U ratio. These ages will be used to discuss the degree of concordance between short-lived nuclides systems and the absolute Pb-Pb clock in early Solar System materials.

Distribution of naturally occurring radionuclides (U, Th) in Timahdit black shale (Morocco).

PubMed

Galindo, C; Mougin, L; Fakhi, S; Nourreddine, A; Lamghari, A; Hannache, H

2007-01-01

Attention has been focused recently on the use of Moroccan black oil shale as the raw material for production of a new type of adsorbent and its application to U and Th removal from contaminated wastewaters. The purpose of the present work is to provide a better understanding of the composition and structure of this shale and to determine its natural content in uranium and thorium. A black shale collected from Timahdit (Morocco) was analyzed by powder X-ray diffraction and SEM techniques. It was found that calcite, dolomite, quartz and clays constitute the main composition of the inorganic matrix. Pyrite crystals are also present. A selective leaching procedure, followed by radiochemical purification and alpha-counting, was performed to assess the distribution of naturally occurring radionuclides. Leaching results indicate that 238U, 235U, 234U, 232Th, 230Th and 228Th have multiple modes of occurrence in the shale. U is interpreted to have been concentrated under anaerobic conditions. An integrated isotopic approach showed the preferential mobilization of uranium carried by humic acids to carbonate and apatite phases. Th is partitioned between silicate minerals and pyrite.

The detailed analysis of natural radionuclides dissolved in spa waters of the Kłodzko Valley, Sudety Mountains, Poland.

PubMed

Walencik-Łata, A; Kozłowska, B; Dorda, J; Przylibski, T A

2016-11-01

A survey was conducted to measure natural radioactivity in spa waters from the Kłodzko Valley. The main goal of this study was to determine the activity concentration of uranium, radium and radon isotopes in the investigated groundwaters. Samples were collected several times from 35 water intakes from 5 spas and 2 mineral water bottling plants. The authors examined whether the increased gamma radiation background, as well as the elevated values of radium and uranium content in reservoir rocks, have a significant impact on the natural radioactivity of these waters. The second objective of this research was to provide information about geochemistry of U, Ra, Rn radionuclides and the radiological and chemical risks incurred by ingestion of isotopes with drinking water. On the basis of results obtained, it is feasible to assess the health hazard posed by ingestion of natural radioactivity with drinking waters. Moreover, the data yielded by this research may be helpful in the process of verification of the application of these waters in balneotherapy. In addition, annual effective radiation doses resulting from the isotopes consumption were calculated on the basis of the evaluated activity concentrations. In dose assessment for uranium and radium isotopes, the authors provided values for different human age groups. The obtained uranium content in the investigated waters was compared with the currently valid regulations concerning the quality of drinking water. Based on the activity concentrations data, the activity isotopic ratios (234)U/(238)U, (226)Ra/(238)U, (222)Rn/(238)U, (222)Rn/(226)Ra and the correlations between radionuclides content were then examined. In brief, it may be concluded on the basis of the obtained results that radon solubility is inversely proportional to radium and uranium dissolution in environmental water circulation. The presented study allows conclusions to be drawn on the radionuclide circulation among different environmental biota: from lithosphere through hydrosphere to biosphere. Copyright © 2016 Elsevier B.V. All rights reserved.

The Effect of Early Diagenesis on the 238U/235U Ratio of Platform Carbonates.

NASA Astrophysics Data System (ADS)

Tissot, F.; Chen, C.; Go, B. M.; Naziemiec, M.; Healy, G.; Swart, P. K.; Dauphas, N.

2017-12-01

In the past 15 years, the so-called non-traditional stable isotopes systems (e.g., Mg, Fe, Mo, U) have emerged as powerful tracers of both high-T and low-T geochemical processes (e.g., [1]). Of particular interest for paleoredox studies is the ratio of "stable" isotopes of U (238U/235U), which has the potential to track the global extent of oceanic anoxia (e.g., [2, 3]). Indeed, in the modern ocean, U exists in two main oxidation states, soluble U6+ and insoluble U4+, and has a mean residence time of 400 kyr ([4]), much longer than the global ocean mixing time (1-2 kyr). As such the salinity-normalized ocean is homogeneous with regards to both U concentrations and isotopes (δ238USW = -0.392±0.005 ‰, [2]). The value of δ238USW at any given time is therefore the balance between U input to the ocean, mainly from rivers, and U removal, mostly into biogenic carbonates, anoxic/euxinic sediments and suboxic/hypoxic sediments (e.g., [2, 5]). Because the 238U/235U ratio of the past ocean cannot be measured directly, it has to be estimated from the measurement of the 238U/235U ratio of a sedimentary rock and assuming a constant fractionation factor. Carbonates appear as a promising record since they span most of Earth's history, and the δ238U values of modern primary carbonate precipitates and well-preserved fossil aragonitic coral up to 600 ka are indistinguishable from that of seawater (e.g., [2, 6, 7]). Yet, the effect of secondary processes on the δ238U values of non-coral carbonates, which represent the bulk of the rock record, has only been studied in a handful of shallow samples (down to 40cm, [6]) and remains poorly understood. To investigate the effect of early diagenesis on the 238U/235U ratio of carbonates on the 30kyr to 1Myr timescale, we measured δ13C, δ18O, and δ238U in samples from a 220m long drill core from the Bahamas carbonate platform. In order to separate lattice bound U from secondary U we developed a leaching protocol applicable to carbonate of all ages. We find that early diagenesis results in a 0 to +0.50 ‰ offset between the δ238U of carbonates and that of seawater. [1] Teng et al (2017) RiMG 82. [2] Tissot & Dauphas (2015) GCA 167. [3] Andersen et al. (2016) Chem. Geol. 420. [4] Ku et al (1977) Deep-Sea Research 24. [5] Dunk et al (2002) Chem. Geol. 190. [6] Romaniello et al (2013) Chem. Geol. 362. [7] Andersen et al. (2014) EPSL 400.

Diagenesis of fossil coral skeletons: Correlation between trace elements, textures, and 234U /238U

NASA Astrophysics Data System (ADS)

Bar-Matthews, M.; Wasserburg, G. J.; Chen, J. H.

1993-01-01

A comparative study of Pleistocene fossil coral skeletons and of modern coral skeletons was carried out using petrographie and trace element analyses on a suite of Pleistocene samples that had previously been studied for 234U, 230Th, and U- 230Th ages ( CHEN et al. 1991). Evidence of a range of diagenetic changes can be recognized by optical (OM) and scanning electron microscopy (SEM). The normal texture exhibited by modern corals under OM consists of fine needles of aragonite forming a radial-fibrous pattern around a central dark line (center of calcification). This pattern can also be seen in many fossil corals. In most cases, the central dark line partially disappears during diagenesis, the radialfibrous pattern is obscured, and there is a distinct coarsening of the radial fabric of aragonite to unoriented platy or equant aragonite crystals. SEM images show diagenetic textures ranging from dense structureless images of the coralline matrix, with sharp boundaries at the septa walls, to the development of (1) a patchy distribution of dissolution micropores partially filled with aragonite fibers in the matrix, (2)aragonite needles coming from selvages in the septa walls which radiate into the septa voids. Using an electron microprobe and SEM, concentrations of Na, S, Sr, and Mg were measured. No other trace elements were detected. Na, S, and Mg contents of the matrix, the fibrous micropores, and radiating needles are highly variable and well correlated. High concentrations of Na, S, and Mg were found in modern living corals with lower concentrations in fossil corals and fibrous micropores, and the lowest value in the radiating needles. The reason for the correlations of Na, S, and Mg and crystal chemistry and the response to diagenesis of these trace elements is not understood. The average concentrations of Na, S, and Mg for each sample, when plotted against the whole coral initial δ 234U, are generally correlated ( CHEN et al., 1991). As all these diagenetic changes involve the recrystallization and deposition of aragonite, we infer that the geologic site of diagenesis both for forming the secondary aragonitic phases and for the enhancement of the 234U content in the fossil corals was the marine environment. It is possible that the textural and Na, S, and Mg trace element contents of fossil corals be used to ascertain the reliability of fossil coral skeletons for U- 230Th dating. The basic problem of identifying a priori unaltered coral skeletons for 230Th dating is not yet resolved.

Origin and transport of (238)U and (226)Ra in riverine, estuarine and marine sediments of the Krka River, Croatia.

PubMed

Cukrov, Neven; Mlakar, Marina; Cuculić, Vlado; Barisić, Delko

2009-06-01

Spatial distribution of (238)U and (226)Ra activities in sediment columns along the Krka River and estuary, were studied using gamma spectrometry. Markedly different (238)U and (226)Ra activities between riverine, estuarine and marine sediments were observed. Distribution of these radionuclides, as well as their anthropogenic and natural origin, was evaluated by activity measurements, taking into account sedimentation rates estimated by (137)Cs distribution in sediment columns. Naturally present (238)U and (226)Ra activities were highest in riverine and lowest in marine sediments. (238)U and (226)Ra activities in historic riverine sediments revealed anthropogenic influence from town of Knin, which diminished for 15-20% in 1990s due to warfare that caused stop of industrial, agricultural and transport activities. Drainage of the flysch material naturally elevates (238)U and (226)Ra activities in the vicinity of its inflow in the upper part of estuary. (238)U and (226)Ra from the phosphate ore discharge in the port of Sibenik did not spread further in estuary, which was also confirmed by (238)U and (226)Ra activities detected in Mytilus sp. mussels' tissue.

Solubility of 238U radionuclide from various types of soil in synthetic gastrointestinal fluids using "US in vitro" digestion method

NASA Astrophysics Data System (ADS)

Rashid, Nur Shahidah Abdul; Sarmani, Sukiman; Majid, Amran Ab.; Mohamed, Faizal; Siong, Khoo Kok

2015-04-01

238U radionuclide is a naturally occuring radioactive material that can be found in soil. In this study, the solubility of 238U radionuclide obtained from various types of soil in synthetic gastrointestinal fluids was analysed by "US P in vitro" digestion method. The synthetic gastrointestinal fluids were added to the samples with well-ordered, mixed throughly and incubated according to the human physiology digestive system. The concentration of 238U radionuclide in the solutions extracted from the soil was measured using Induced Coupling Plasma Mass Spectrometer (ICP-MS). The concentration of 238U radionuclide from the soil samples in synthetic gastrointestinal fluids showed different values due to different homogenity of soil types and chemical reaction of 238U radionuclide. In general, the solubility of 238U radionuclide in gastric fluid was higher (0.050 - 0.209 ppm) than gastrointestinal fluids (0.024 - 0.050 ppm). It could be concluded that the US P in vitro digestion method is practicle for estimating the solubility of 238U radionuclide from soil materials and could be useful for monitoring and risk assessment purposes applying to environmental, health and contaminated soil samples.

Enhanced techniques for the measurement of ultra-low level (pg and fg) actinide analysis by ICP-MS for forensic and geologic applications

NASA Astrophysics Data System (ADS)

Pollington, A. D.; Kinman, W.; Hanson, S. K.

2014-12-01

Recent advances in mass spectrometry have led to an improved ability to measure high precision isotope ratios at increasingly low analyte concentrations. Combining techniques for enhanced ionization with better counting of small ion beams, we routinely measure isotope ratios on 100's of pg uranium samples and ≤10 pg plutonium samples with relative standard deviations of 1‰ on major isotope ratios and 10‰ on minor ratios achievable. With slightly larger samples (≤1 ng total U), these precisions can be as low as 0.01‰ (10 ppm) and 1‰ respectively. These techniques can be applied to both nuclear forensics questions where only a small amount of sample is available, as well as geologic questions such as U-Pb or U-Th disequilibrium geochronology from either single small crystals, or microsampled domains from within a heterogeneous sample. The analytical setup is a Cetac Aridus II desolvating nebulizer interfaced with a ThermoScientific Neptune Plus equipped with a jet-type sample cone and x-type skimmer cone. The combination of the desolvating nebulizer with the enhanced cone setup leads to an increase in sensitivity on the order of 10x that of a standard glass spray chamber (~1000V/ppm U). The Neptune Plus is equipped with 9 Faraday cups and 5 electron multipliers (two behind RPQ energy filters for improved abundance sensitivtiy). This allows for the simultaneous collection of all isotopes of either U or Pu with a combination of Faraday cups (e.g., 235U and 238U) and electron multipliers (e.g., 234U and 236U) with other configurations also available (e.g., 235U and 238U can instead be measured on electron multipliers in small samples). As sample sizes get small, the contributions from environmental blanks, as well as interfering species, become increasing concerns. In this study, we will present data on efforts to minimize the contribution of environmental U using scaled down chemical procedures as well as the effect of polyatomic species on the precision and accuracy of actinide isotope measurements and what procedures can be applied to minimize interferences.

The 238U/235U isotope ratio of the Earth and the solar system: Constrains from a gravimetrically calibrated U double spike and implications for absolute Pb-Pb ages

NASA Astrophysics Data System (ADS)

Weyer, Stefan; Noordmann, Janine; Brennecka, Greg; Richter, Stephan

2010-05-01

The ratio of 238U and 235U, the two primordial U isotopes, has been assumed to be constant on Earth and in the solar system. The commonly accepted value for the 238U/235U ratio, which has been used in Pb-Pb dating for the last ~ 30 years, was 137.88. Within the last few years, it has been shown that 1) there are considerable U isotope variations (~1.3‰) within terrestrial material produced by isotope fractionation during chemical reactions [1-3] and 2) there are even larger isotope variations (at least 3.5‰) in calcium-aluminum-rich inclusions (CAIs) in meoteorites that define the currently accepted age of the solar system [4]. These findings are dramatic for geochronology, as a known 238U/235U is a requirement for Pb-Pb dating, the most precise dating technique for absolute ages. As 238U/235U variations can greatly affect the reported absolute Pb-Pb age, understanding and accurately measuring variation of the 238U/235U ratio in various materials is critical, With these new findings, the questions also arises of "How well do we know the average U isotope composition of the Earth and the solar system?" and "How accurate can absolute Pb-Pb ages be?" Our results using a gravimetrically calibrated 233U/236U double spike IRMM 3636 [5] indicate that the U standard NBL 950a, which was commonly used to define the excepted "natural" 238U/235U isotope ratio, has a slightly lower 238U/235U of 137.836 ± 0.024. This value is indistinguishable from the U isotope compositions for NBL 960 and NBL112A, which have been determined by several laboratories, also using the newly calibrated U double spike IRMM 3636 [6]. These findings provide new implications about the average U isotope composition of the Earth and the solar system. Basalts display a very tight range of U isotope variations (~0.25-0.32‰ relative to SRM 950a). Their U isotope composition is also very similar to that of chondrites [4], which however appear to show a slightly larger spread. Accepting terrestrial basalts to be the best representation of the U isotope composition of the Earth and the solar system, and the new 238U/235U for SRM 950a of 137.836, this would result in an average 238U/235U for the Earth and the solar system of ~ 137.80. The effect of a revised 238U/235U ratio on Pb-Pb ages is age dependent. It results in an age overestimation of ~0.8 Ma for the age of the solar system and up to 1.5 Ma for very young material (with bulk Earth U isotope composition). [1] Stirling, C.H., Andersen, M.B., Potter, E.-K., et al. (2007) EPSL 264, 208-225; [2] Weyer, S., Anbar, A. D., Gerdes, A., et al. (2008) GCA 72, 345-359. [3] Bopp, C.H., Lundstrom, C.C., Johnsons, T.M., Glessner, J.G. (2009) Geology 37, 611-614. [4] Brennecka, G.A., Weyer, S., Wadhwa, et al. (2010) Science, 327, p. 449. [5] Richter, S., Alonzo-Munoz, A., Eykens, R., et al. (2008) IJMS 269, 145-148. [6] Richter, S., et al. EGU meeting 2010.

238U and 235U isotope fractionation upon oxidation of uranium-bearing rocks by fracture waters

NASA Astrophysics Data System (ADS)

Chernyshev, I. V.; Golubev, V. N.; Chugaev, A. V.; Mandzhieva, G. V.

2016-10-01

The variations in 238U/235U values accompanying mobilization of U by fracture waters from uranium-bearing rocks, in which U occurs as a fine impregnation of oxides and silicates, were studied by the high-precision (±0.07‰) MC-ICP-MS method. Transition of U into the aqueous phase in the oxidized state U(VI) is accompanied by its isotope fractionation with enrichment of dissolved U(VI) in the heavy isotope 238U up to 0.32‰ in relation to the composition of the solid phases. According to the sign, this effect is consistent with the tendency of the behavior of 238U and 235U upon interaction of river waters with rocks of the catchment areas [11] and with the effect observed during oxidation of uraninite by the oxygen-bearing NaHCO3 solution [12].

Health implications of radionuclide levels in cattle raised near U mining and milling facilities in Ambrosia Lake, New Mexico

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lapham, S.C.; Millard, J.B.; Samet, J.M.

1989-03-01

This study was conducted to determine radionuclide tissue levels in cattle raised near U mining and milling facilities. Ambrosia Lake, New Mexico, has been the site of extensive U mining for 30 y and contains several underground U mines, a processing mill, and two large U tailings piles. Ten cows were purchased from two grazing areas in Ambrosia Lake and ten control animals were purchased from Crownpoint, New Mexico. Muscle, liver, kidney, and bone tissue taken from these animals, and environmental samples, including water, grasses and soil collected from the animals' grazing areas, were analyzed for /sup 238/U, /sup 234/U,more » /sup 230/Th, /sup 226/Ra, /sup 210/Pb, and /sup 210/Po. Mean radionuclide levels in cattle tissue and environmental samples from Ambrosia Lake were higher in almost every comparison than those found in respective controls. Liver and kidney tissues were particularly elevated in /sup 226/Ra and /sup 210/Po. Radiation dose commitments from eating cattle tissue with these radionuclide concentrations were calculated. We concluded that the health risk to the public from eating exposed cattle is minimal, unless large amounts of this tissue, especially liver and kidney, are ingested.« less

New frontiers in coral geochronology: advancing the state of the art

NASA Astrophysics Data System (ADS)

Thompson, William G.

2010-05-01

New developments in mass spectrometry and a better understanding of open-system processes are ushering in a new era of precision and accuracy in coral geochronology. An effort is underway to develop a uniform set of reference materials and reporting standards to assure age comparability between laboratories and eliminate inter-laboratory and age interpretation biases. PALSEA is a PAGES/IMAGES working group that aims to extract information about ice sheet response to temperature change by examining the history of sea during past interglacials. As reef-building corals are one of the primary archives of past sea levels, the U-series coral dating community is well represented in this group. During workshop discussions, it became clear that further progress on the sea level problem requires engaging the coral dating community in a cooperative standardization effort. Improvements in analytical precision continue to extend the potential precision and range of the U-Th chronometer. As a result, assuring comparability of ages reported by different labs becomes a crucial issue. Ideally, all measurements should be traceable to the same set of reference standards. Unfortunately, internationally recognized standards are not currently available. A widely used U/Th uraninite standard, HU-1, is no longer be suitable, as different aliquots have different isotope ratios and the assumption of radioactive equilibrium no longer appears valid when measured at current levels of precision. The time is ripe for the development of new reference standards. A strategy for their production and distribution has been initiated in collaboration with the NERC Isotope Geosciences Laboratory, UK, and drawing on the experiences of the EARTHTIME initiative (http://www.earth-time.org). Quaternary sea level data is presently scattered across the scientific literature with widely varying reporting formats, screening and correction criteria, and decay constants. Stratigraphic information is often incomplete, and elevations are not tied to consistent benchmarks. It would be highly desirable to compile existing data in a uniform format that can be made available to the wider community, and to adopt a uniform set of standards for future data reporting. While best practices for sample screening and/or age correction are still keenly debated, reported ages depend heavily on assumptions about the 234U/238U history of seawater over the last 800 thousand years. A standard history of ocean 234U/238U for quality and correction criteria, with associated error estimates, would make ages reported by different labs more directly comparable. Data reduction and archiving software has been developed as part of the EARTHTIME project, and discussions are underway to adapt this software for the U-Th chronometer. Standardized reporting through data reduction and databasing software has great potential to make U-series dating of coral sea-level indicators more useful and accessible to the wider paleoclimate community.

Entry of uranium, thorium, and radium isotopes into plants from soils and fertilizers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shishkunova, L.V.; Grashchenko, S.M.; Strukov, V.N.

1989-01-01

We studied the effect of phosphorus fertilizers on the entry of /sup 238/U, /sup 234/U, /sup 228/Th, /sup 230/Th, /sup 232/Th, and /sup 226/Ra into crops from soils. Also examined was plant uptake of radionuclides originating from the fertilizers. Raising the phosphate content by incorporating the fertilizers into certain soils changed the ratio of the amount of radionuclide available to a plant to that fixed in the soil. A specific case was the addition of 4000 kg/ha of ammophos to soddy podzolic soils, which raised the thorium isotope buildup factor by 2 to 3. The uptake of thorium from ammophosmore » by plants, as measured by the entry ratio, was a hundred times lower than from the soils.« less

Monte Carlo analysis of TRX lattices with ENDF/B version 3 data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hardy, J. Jr.

1975-03-01

Four TRX water-moderated lattices of slightly enriched uranium rods have been reanalyzed with consistent ENDF/B Version 3 data by means of the full-range Monte Carlo program RECAP. The following measured lattice parameters were studied: ratio of epithermal-to-thermal $sup 238$U capture, ratio of epithermal- to-thermal $sup 235$U fissions, ration of $sup 238$U captures to $sup 235$U fissions, ratio of $sup 238$U fissions to $sup 235$U fissions, and multiplication factor. In addition to the base calculations, some studies were done to find sensitivity of the TRX lattice parameters to selected variations of cross section data. Finally, additional experimental evidence is afforded bymore » effective $sup 238$U capture integrals for isolated rods. Shielded capture integrals were calculated for $sup 238$U metal and oxide rods. These are compared with other measurements. (auth)« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rashid, Nur Shahidah Abdul; Sarmani, Sukiman; Majid, Amran Ab.

238U radionuclide is a naturally occuring radioactive material that can be found in soil. In this study, the solubility of 238U radionuclide obtained from various types of soil in synthetic gastrointestinal fluids was analysed by “US P in vitro” digestion method. The synthetic gastrointestinal fluids were added to the samples with well-ordered, mixed throughly and incubated according to the human physiology digestive system. The concentration of 238U radionuclide in the solutions extracted from the soil was measured using Induced Coupling Plasma Mass Spectrometer (ICP-MS). The concentration of 238U radionuclide from the soil samples in synthetic gastrointestinal fluids showed different valuesmore » due to different homogenity of soil types and chemical reaction of 238U radionuclide. In general, the solubility of 238U radionuclide in gastric fluid was higher (0.050 – 0.209 ppm) than gastrointestinal fluids (0.024 – 0.050 ppm). It could be concluded that the US P in vitro digestion method is practicle for estimating the solubility of 238U radionuclide from soil materials and could be useful for monitoring and risk assessment purposes applying to environmental, health and contaminated soil samples.« less

High resolution isotopic analysis of U-bearing particles via fusion of SIMS and EDS images

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tarolli, Jay G.; Naes, Benjamin E.; Garcia, Benjamin J.

Image fusion of secondary ion mass spectrometry (SIMS) images and X-ray elemental maps from energy-dispersive spectroscopy (EDS) was performed to facilitate the isolation and re-analysis of isotopically unique U-bearing particles where the highest precision SIMS measurements are required. Image registration, image fusion and particle micromanipulation were performed on a subset of SIMS images obtained from a large area pre-screen of a particle distribution from a sample containing several certified reference materials (CRM) U129A, U015, U150, U500 and U850, as well as a standard reference material (SRM) 8704 (Buffalo River Sediment) to simulate particles collected on swipes during routine inspections ofmore » declared uranium enrichment facilities by the International Atomic Energy Agency (IAEA). In total, fourteen particles, ranging in size from 5 – 15 µm, were isolated and re-analyzed by SIMS in multi-collector mode identifying nine particles of CRM U129A, one of U150, one of U500 and three of U850. These identifications were made within a few percent errors from the National Institute of Standards and Technology (NIST) certified atom percent values for 234U, 235U and 238U for the corresponding CRMs. This work represents the first use of image fusion to enhance the accuracy and precision of isotope ratio measurements for isotopically unique U-bearing particles for nuclear safeguards applications. Implementation of image fusion is essential for the identification of particles of interests that fall below the spatial resolution of the SIMS images.« less

Concentrations and activity ratios of uranium isotopes in groundwater from Doñana National Park, South of Spain

NASA Astrophysics Data System (ADS)

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

2008-08-01

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

28 CFR 2.38 - Community supervision by U.S. Probation Officers.

Code of Federal Regulations, 2011 CFR

2011-07-01

... 28 Judicial Administration 1 2011-07-01 2011-07-01 false Community supervision by U.S. Probation Officers. 2.38 Section 2.38 Judicial Administration DEPARTMENT OF JUSTICE PAROLE, RELEASE, SUPERVISION AND... § 2.38 Community supervision by U.S. Probation Officers. (a) Pursuant to sections 3655 and 4203(b)(4...

28 CFR 2.38 - Community supervision by U.S. Probation Officers.

Code of Federal Regulations, 2013 CFR

2013-07-01

... 28 Judicial Administration 1 2013-07-01 2013-07-01 false Community supervision by U.S. Probation Officers. 2.38 Section 2.38 Judicial Administration DEPARTMENT OF JUSTICE PAROLE, RELEASE, SUPERVISION AND... § 2.38 Community supervision by U.S. Probation Officers. (a) Pursuant to sections 3655 and 4203(b)(4...

28 CFR 2.38 - Community supervision by U.S. Probation Officers.

Code of Federal Regulations, 2010 CFR

2010-07-01

... 28 Judicial Administration 1 2010-07-01 2010-07-01 false Community supervision by U.S. Probation Officers. 2.38 Section 2.38 Judicial Administration DEPARTMENT OF JUSTICE PAROLE, RELEASE, SUPERVISION AND... § 2.38 Community supervision by U.S. Probation Officers. (a) Pursuant to sections 3655 and 4203(b)(4...

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 preferentially adsorbed [5]. Whether plankton mediated chemical reduction or scavenging causes this fractionation will be further investigated by leaching experiments on sediment trap samples. By contrast, weak acidic leachates (at pH 6) of suboxic bottom sediments, tend towards higher δ238U values. For oxic sediments, U contents of this fraction were below detection limit. Stronger leaching at pH 3 removed most of the uranium from suboxic and oxic sediments. For oxic sediments, this fraction yields the seawater δ238U signature, while the U released from the suboxic sample is about 0.2‰ heavier. This matches the value for previously reported bulk analyses of suboxic sediments [1] implying that the reduced sedimentary U is released by this treatment,. Major and trace element analyses and XRD patterns will help relating this fraction to a specific mineral or reactive phase. [1] Weyer et al. (2007) GCA 72, 345-399. [2] Stirling et al. (2007) EPSL 264, 208-225. [3] Schauble (2007) GCA 71, 2170-2189. [4] Rademacher et al. (2006) Environ. Sci. Technol. 40,6943-6948. [5] Wasylenki (2009) GCA A1419.

Investigating uranium distribution in surface sediments and waters: a case study of contamination from the Juniper Uranium Mine, Stanislaus National Forest, CA.

PubMed

Kayzar, Theresa M; Villa, Adam C; Lobaugh, Megan L; Gaffney, Amy M; Williams, Ross W

2014-10-01

The uranium concentrations and isotopic compositions of waters, sediment leachates and sediments from Red Rock Creek in the Stanislaus National Forest of California were measured to investigate the transport of uranium from a point source (the Juniper Uranium Mine) to a natural surface stream environment. The ((234)U)/((238)U) composition of Red Rock Creek is altered downstream of the Juniper Mine. As a result of mine-derived contamination, water ((234)U)/((238)U) ratios are 67% lower than in water upstream of the mine (1.114-1.127 ± 0.009 in the contaminated waters versus 1.676 in the clean branch of the stream), and sediment samples have activity ratios in equilibrium in the clean creek and out of equilibrium in the contaminated creek (1.041-1.102 ± 0.007). Uranium concentrations in water, sediment and sediment leachates are highest downstream of the mine, but decrease rapidly after mixing with the clean branch of the stream. Uranium content and compositions of the contaminated creek headwaters relative to the mine tailings of the Juniper Mine suggest that uranium has been weathered from the mine and deposited in the creek. The distribution of uranium between sediment surfaces (leachable fraction) and bulk sediment suggests that adsorption is a key element of transfer along the creek. In clean creek samples, uranium is concentrated in the sediment residues, whereas in the contaminated creek, uranium is concentrated on the sediment surfaces (∼70-80% of uranium in leachable fraction). Contamination only exceeds the EPA maximum contaminant level (MCL) for drinking water in the sample with the closest proximity to the mine. Isotopic characterization of the uranium in this system coupled with concentration measurements suggest that the current state of contamination in Red Rock Creek is best described by mixing between the clean creek and contaminated upper branch of Red Rock Creek rather than mixing directly with mine sediment. Published by Elsevier Ltd.

Investigating uranium distribution in surface sediments and waters: a case study of contamination from the Juniper Uranium Mine, Stanislaus National Forest, CA

DOE PAGES

Kayzar, Theresa M.; Villa, Adam C.; Lobaugh, Megan L.; ...

2014-06-07

The uranium concentrations and isotopic compositions of waters, sediment leachates and sediments from Red Rock Creek in the Stanislaus National Forest of California were measured to investigate the transport of uranium from a point source (the Juniper Uranium Mine) to a natural surface stream environment. Furthermore, we alter the (234U)/(238U) composition of Red Rock Creek downstream of the Juniper Mine. As a result of mine-derived contamination, water (234U)/(238U) ratios are 67% lower than in water upstream of the mine (1.114–1.127 ± 0.009 in the contaminated waters versus 1.676 in the clean branch of the stream), and sediment samples have activitymore » ratios in equilibrium in the clean creek and out of equilibrium in the contaminated creek (1.041–1.102 ± 0.007). Uranium concentrations in water, sediment and sediment leachates are highest downstream of the mine, but decrease rapidly after mixing with the clean branch of the stream. Uranium content and compositions of the contaminated creek headwaters relative to the mine tailings of the Juniper Mine suggest that uranium has been weathered from the mine and deposited in the creek. The distribution of uranium between sediment surfaces (leachable fraction) and bulk sediment suggests that adsorption is a key element of transfer along the creek. In clean creek samples, uranium is concentrated in the sediment residues, whereas in the contaminated creek, uranium is concentrated on the sediment surfaces (~70–80% of uranium in leachable fraction). Furthermore, contamination only exceeds the EPA maximum contaminant level (MCL) for drinking water in the sample with the closest proximity to the mine. Isotopic characterization of the uranium in this system coupled with concentration measurements suggest that the current state of contamination in Red Rock Creek is best described by mixing between the clean creek and contaminated upper branch of Red Rock Creek rather than mixing directly with mine sediment.« less

Using 238U/235U ratios to understand the formation and oxidation of reduced uranium solids in naturally reduced zones

NASA Astrophysics Data System (ADS)

Jemison, N.; Johnson, T. M.; Druhan, J. L.; Davis, J. A.

2016-12-01

Uranium occurs in groundwater primarily as soluble and mobile U(VI), which can be reduced to immobile U(IV), often observed in sediments as uraninite. Numerous U(VI)-contaminated sites, such as the DOE field site in Rifle, CO, contain naturally reduced zones (NRZ's) that have relatively high concentrations of organic matter. Reduction of heavy metals occurs within NRZ's, producing elevated concentrations of iron sulfides and U(IV). Slow, natural oxidation of U(IV) from NRZ's may prolong U(VI) contamination of groundwater. The reduction of U(VI) produces U(IV) with a higher 238U/235U ratio. Samples from two NRZ sediment cores recovered from the Rifle site revealed that the outer fringes of the NRZ contain U(IV) with a high 238U/235U ratio, while lower values are observed in the center . We suggest that as aqueous U(VI) was reduced in the NRZ, it was driven to lower 238U/235U values, such that U(IV) formed in the core of the NRZ reflects a lower 238U/235U. Two oxidation experiments were conducted by injecting groundwater containing between 14.9 and 21.2 mg/L dissolved O2 as an oxidant into the NRZ. The oxidation of U(IV) from this NRZ increased aqueous U(VI) concentrations and caused a shift to higher 238U/235U in groundwater as U(IV) was oxidized primarily on the outer fringes of the NRZ. In total these observations suggest that the stability of solid phase uranium is governed by coupled reaction and transport processes. To better understand various reactive transport scenarios we developed a model for the formation and oxidation of NRZ's utilizing the reactive transport software CrunchTope. These simulations suggest that the development of isotopically heterogeneous U(IV) within NRZ's is largely controlled by permeability of the NRZ and the U(VI) reduction rate. Oxidation of U(IV) from the NRZ's is constrained by the oxidation rate of U(IV) as well as iron sulfides, which can prevent oxidation of U(IV) by scavenging dissolved oxygen.

Modern U-Pb chronometry of meteorites: advancing to higher time resolution reveals new problems

USGS Publications Warehouse

Amelin, Y.; Connelly, J.; Zartman, R.E.; Chen, J.-H.; Gopel, C.; Neymark, L.A.

2009-01-01

In this paper, we evaluate the factors that influence the accuracy of lead (Pb)-isotopic ages of meteorites, and may possibly be responsible for inconsistencies between Pb-isotopic and extinct nuclide timescales of the early Solar System: instrumental mass fractionation and other possible analytical sources of error, presence of more than one component of non-radiogenic Pb, migration of ancient radiogenic Pb by diffusion and other mechanisms, possible heterogeneity of the isotopic composition of uranium (U), uncertainties in the decay constants of uranium isotopes, possible presence of "freshly synthesized" actinides with short half-life (e.g. 234U) in the early Solar System, possible initial disequilibrium in the uranium decay chains, and potential fractionation of radiogenic Pb isotopes and U isotopes caused by alpha-recoil and subsequent laboratory treatment. We review the use of 232Th/238U values to assist in making accurate interpretations of the U-Pb ages of meteorite components. We discuss recently published U-Pb dates of calcium-aluminum-rich inclusions (CAIs), and their apparent disagreement with the extinct nuclide dates, in the context of capability and common pitfalls in modern meteorite chronology. Finally, we discuss the requirements of meteorites that are intended to be used as the reference points in building a consistent time scale of the early Solar System, based on the combined use of the U-Pb system and extinct nuclide chronometers.

Result Summary for the Area 5 Radioactive Waste Management Site Performance Assessment Model Version 4.110

DOE Office of Scientific and Technical Information (OSTI.GOV)

NSTec Environmental Management

2011-07-20

Results for Version 4.110 of the Area 5 Radioactive Waste Management Site (RWMS) performance assessment (PA) model are summarized. Version 4.110 includes the fiscal year (FY) 2010 inventory estimate, including a future inventory estimate. Version 4.110 was implemented in GoldSim 10.11(SP4). The following changes have been implemented since the last baseline model, Version 4.105: (1) Updated the inventory and disposal unit configurations with data through the end of FY 2010. (1) Implemented Federal Guidance Report 13 Supplemental CD dose conversion factors (U.S. Environmental Protection Agency, 1999). Version 4.110 PA results comply with air pathway and all-pathways annual total effective dosemore » (TED) performance objectives (Tables 2 and 3, Figures 1 and 2). Air pathways results decrease moderately for all scenarios. The time of the maximum for the air pathway open rangeland scenario shifts from 1,000 to 100 years (y). All-pathways annual TED increases for all scenarios except the resident scenario. The maximum member of public all-pathways dose occurs at 1,000 y for the resident farmer scenario. The resident farmer dose was predominantly due to technetium-99 (Tc-99) (82 percent) and lead-210 (Pb-210) (13 percent). Pb-210 present at 1,000 y is produced predominantly by radioactive decay of uranium-234 (U-234) present at the time of disposal. All results for the postdrilling and intruder-agriculture scenarios comply with the performance objectives (Tables 4 and 5, Figures 3 and 4). The postdrilling intruder results are similar to Version 4.105 results. The intruder-agriculture results are similar to Version 4.105, except for the Pit 6 Radium Disposal Unit (RaDU). The intruder-agriculture result for the Shallow Land Burial (SLB) disposal units is a significant fraction of the performance objective and exceeds the performance objective at the 95th percentile. The intruder-agriculture dose is due predominantly to Tc-99 (75 percent) and U-238 (9.5 percent). The acute intruder scenario results comply with all performance objectives (Tables 6 and 7, Figures 5 and 6). The acute construction result for the SLB disposal units decreases significantly with this version. The maximum acute intruder dose occurs at 1,000 y for the SLB disposal units under the acute construction scenario. The acute intruder dose is caused by multiple radionuclides including U-238 (31 percent), Th-229 (28 percent), plutonium-239 (8.6 percent), U-233 (7.8 percent), and U-234 (6.7 percent). All results for radon-222 (Rn-222) flux density comply with the performance objective (Table 8, Figure 7). The mean Pit 13 RaDU flux density is close to the 0.74 Bq m{sup -2} s{sup -1} limit.« less

A database of radionuclide activity and metal concentrations for the Alligator Rivers Region uranium province.

PubMed

Doering, Che; Bollhöfer, Andreas

2016-10-01

This paper presents a database of radionuclide activity and metal concentrations for the Alligator Rivers Region (ARR) uranium province in the Australian wet-dry tropics. The database contains 5060 sample records and 57,473 concentration values. The data are for animal, plant, soil, sediment and water samples collected by the Environmental Research Institute of the Supervising Scientist (ERISS) as part of its statutory role to undertake research and monitoring into the impacts of uranium mining on the environment of the ARR. Concentration values are provided in the database for 11 radionuclides ( 227 Ac, 40 K, 210 Pb, 210 Po, 226 Ra, 228 Ra, 228 Th, 230 Th, 232 Th, 234 U, 238 U) and 26 metals (Al, As, Ba, Ca, Cd, Co, Cr, Cu, Fe, Hg, K, Mg, Mn, Na, Ni, P, Pb, Rb, S, Sb, Se, Sr, Th, U, V, Zn). Potential uses of the database are discussed. Crown Copyright © 2016. Published by Elsevier Ltd. All rights reserved.

Radiation Doses to Members of the U.S. Population from Ubiquitous Radionuclides in the Body: Part 1, Autopsy and In Vivo Data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Watson, David J.; Strom, Daniel J.

This paper is part one of a three-part series investigating annual effective doses to residents of the United States from intakes of ubiquitous radionuclides, including radionuclides occurring naturally, radionuclides whose concentrations are technologically enhanced, and anthropogenic radionuclides. This series of papers explicitly excludes intakes from inhaling 222Rn, 220Rn, and their short-lived decay products; it also excludes intakes of radionuclides in occupational and medical settings. The goal of part one of this work was to review, summarize, and characterize all published and some unpublished data for U.S. residents on ubiquitous radionuclide concentrations in tissues and organs. Forty-five papers and reports weremore » obtained and their data reviewed, and three data sets were obtained via private communication. The 45 radionuclides of interest are the 238U series (14 nuclides), the actinium series (headed by 235U; 11 nuclides), and the 232Th series (11 nuclides); primordial radionuclides 87Rb and 40 K; cosmogenic and fallout radionuclides 14C and 3H; and purely anthropogenic radionuclides 137Cs-137mBa, 129I, and 90Sr-90Y. Measurements judged to be relevant were available for only 15 of these radionuclides: 238U, 235U, 234U, 232Th, 230Th, 228Th, 228Ra, 226Ra, 210Pb, 210Po, 137Cs, 87Rb, 40K, 14C, and 3H. Recent and relevant measurements were not available for 129I and 90Sr-90Y. A total of 11,714 radionuclide concentration measurements were found in one or more tissues or organs from 14 States. Data on age, sex, geographic locations, height, and weight of subjects were available only sporadically. Too often authors did not provide meaningful values of uncertainty of measurements so that variability in data sets is confounded with measurement uncertainty. The following papers detail how these shortcomings are overcome to achieve the goals of the three-part series.« less

Uranium uptake history, open-system behaviour and uranium-series ages of fossil Tridacna gigas from Huon Peninsula, Papua New Guinea

NASA Astrophysics Data System (ADS)

Ayling, Bridget F.; Eggins, Stephen; McCulloch, Malcolm T.; Chappell, John; Grün, Rainer; Mortimer, Graham

2017-09-01

Molluscs incorporate negligible uranium into their skeleton while they are living, with any uranium uptake occurring post-mortem. As such, closed-system U-series dating of molluscs is unlikely to provide reliable age constraints for marine deposits. Even the application of open-system U-series modelling is challenging, because uranium uptake and loss histories can affect time-integrated uranium distributions and are difficult to constrain. We investigate the chemical and isotopic distribution of uranium in fossil Tridacna gigas (giant clams) from Marine Isotope Stage (MIS) 5e (128-116 ka) and MIS 11 (424-374 ka) reefs at Huon Peninsula in Papua New Guinea. The large size of the clams enables detailed chemical and isotopic mapping of uranium using LA-ICPMS and LA-MC-ICPMS techniques. Within each fossil Tridacna specimen, marked differences in uranium concentrations are observed across the three Tridacna growth zones (outer, inner, hinge), with the outer and hinge zones being relatively enriched. In MIS 5e and MIS 11 Tridacna, the outer and hinge zones contain approximately 1 ppm and 5 ppm uranium respectively. In addition to uptake of uranium, loss of uranium appears prevalent, especially in the MIS 11 specimens. The effect of uranium loss is to elevate measured [230Th/238U] values with little effect on [234U/238U] values. Closed-system age estimates are on average 50% too young for the MIS 5e Tridacna, and 25% too young for the MIS 11 Tridacna. A complex, multi-stage uptake and loss history is interpreted for the fossil Tridacna and we demonstrate that they cannot provide independent, reliable geochronological controls on the timing of past reef growth at Huon Peninsula.

Natural radionuclides in lichens, mosses and ferns in a thermal power plant and in an adjacent coal mine area in southern Brazil.

PubMed

Galhardi, Juliana Aparecida; García-Tenorio, Rafael; Díaz Francés, Inmaculada; Bonotto, Daniel Marcos; Marcelli, Marcelo Pinto

2017-02-01

The radio-elements 234 U, 235 U, 238 U, 230 Th, 232 Th and 210 Po were characterized in lichens, mosses and ferns species sampled in an adjacent coal mine area at Figueira City, Paraná State, Brazil, due to their importance for the assessment of human exposure related to the natural radioactivity. The coal is geologically associated with a uranium deposit and has been used as a fossil fuel in a thermal power plant in the city. Samples were initially prepared at LABIDRO (Isotopes and Hydrochemistry Laboratory), UNESP, Rio Claro (SP), Brazil. Then, alpha-spectrometry after several radiochemical steps was used at the Applied Nuclear Physics Laboratories, University of Seville, Seville, Spain, for measuring the activity concentration of the radionuclides. It was 210 Po the radionuclide that most bio-accumulates in the organisms, reaching the highest levels in mosses. The ferns species were less sensitive as bio-monitor than the mosses and lichens, considering polonium in relation to other radionuclides. Fruticose lichens exhibited lower polonium content than the foliose lichens sampled in the same site. Besides biological features, environmental characteristics also modify the radio-elements absorption by lichens and mosses like the type of vegetation covering these organisms, their substrate, the prevailing wind direction, elevation and climatic conditions. Only 210 Po and 238 U correlated in ferns and in soil and rock materials, being particulate emissions from the coal-fired power plant the most probable U-source in the region. Thus, the biomonitors used were able to detect atmospheric contamination by the radionuclides monitored. Copyright © 2016 Elsevier Ltd. All rights reserved.

Biogeochemical aspects of uranium mineralization, mining, milling, and remediation

USGS Publications Warehouse

Campbell, Kate M.; Gallegos, Tanya J.; Landa, Edward R.

2015-01-01

Natural uranium (U) occurs as a mixture of three radioactive isotopes: 238U, 235U, and 234U. Only 235U is fissionable and makes up about 0.7% of natural U, while 238U is overwhelmingly the most abundant at greater than 99% of the total mass of U. Prior to the 1940s, U was predominantly used as a coloring agent, and U-bearing ores were mined mainly for their radium (Ra) and/or vanadium (V) content; the bulk of the U was discarded with the tailings (Finch et al., 1972). Once nuclear fission was discovered, the economic importance of U increased greatly. The mining and milling of U-bearing ores is the first step in the nuclear fuel cycle, and the contact of residual waste with natural water is a potential source of contamination of U and associated elements to the environment. Uranium is mined by three basic methods: surface (open pit), underground, and solution mining (in situ leaching or in situ recovery), depending on the deposit grade, size, location, geology and economic considerations (Abdelouas, 2006). Solid wastes at U mill tailings (UMT) sites can include both standard tailings (i.e., leached ore rock residues) and solids generated on site by waste treatment processes. The latter can include sludge or “mud” from neutralization of acidic mine/mill effluents, containing Fe and a range of coprecipitated constituents, or barium sulfate precipitates that selectively remove Ra (e.g., Carvalho et al., 2007). In this chapter, we review the hydrometallurgical processes by which U is extracted from ore, the biogeochemical processes that can affect the fate and transport of U and associated elements in the environment, and possible remediation strategies for site closure and aquifer restoration.This paper represents the fourth in a series of review papers from the U.S. Geological Survey (USGS) on geochemical aspects of UMT management that span more than three decades. The first paper (Landa, 1980) in this series is a primer on the nature of tailings and radionuclide mobilization from them. The second paper (Landa, 1999) includes coverage of research carried out under the U.S. Department of Energy’s Uranium Mill Tailings Remedial Action Program (UMTRA). The third paper (Landa, 2004) reflects the increased focus of researchers on biotic effects in UMT environs. This paper expands the focus to U mining, milling, and remedial actions, and includes extensive coverage of the increasingly important alkaline in situ recovery and groundwater restoration.

A modern framework for the interpretation of 238U/235U in studies of ancient ocean redox

NASA Astrophysics Data System (ADS)

Andersen, M. B.; Romaniello, S.; Vance, D.; Little, S. H.; Herdman, R.; Lyons, T. W.

2014-08-01

The abundance and isotope composition of redox sensitive elements in ancient sediments are increasingly used to understand the past ocean's geochemical state and the oxygenation history of the Earth. The redox transition of uranium (U) from soluble U+6 to relatively insoluble U+4 and its subsequent incorporation into reduced sediments has been used to deduce the redox state of the oceans in the past. Furthermore, recent analytical improvements have revealed significant 238U/235U fractionation during this redox transition, offering the potential for U isotopes to act as a redox proxy. However, the development of U isotopes as a geochemical tracer requires that U isotope systematics associated with redox changes, are well-characterized. This study focuses on U isotopes in recent sediments from the two largest modern anoxic ocean basins, the Black Sea and the Cariaco Basin, with the aim of advancing our understanding of the U isotope systematics in reducing marine environments. These anoxic sediments have high U accumulation rates and high 238U/235U ratios relative to seawater, in general agreement with a process that accumulates reduced U with a heavy isotopic composition. Using Al and Ca concentrations to correct for detrital and biogenic carbonate-bound U, we estimate the reduced authigenic U accumulated in the sediments and its 238U/235U. These results highlight the importance of isotopic mass balance constraints during diffusive transport and reaction of U from seawater and through pore-water, affecting the observed 238U/235U in sediments. Using these constraints, the average percentages of U depletion from top to bottom of the water column can be estimated, assuming batch-removal of U into anoxic sediments in a restricted basin. Using this framework, 238U/235U in modern anoxic sediments from the Black Sea imply U depletions in the water column of ∼30%, which is close to the observed ∼40% U depletion in the modern Black Sea water column at these depths. Similar U depletion in the water column is estimated from anoxic sediment samples of the Cariaco Basin. These recent anoxic sediments provide a basis for interpreting authigenic 238U/235U in ancient sediments. In particular, such analyses may offer insights, based on mass balance relationships, into whether particular ancient sediments were deposited in an open ocean or restricted basin. As such, this approach may provide key insight into the controls on local versus ocean-scale redox and, in that light, constraints the capacity of other proxies to capture global signals for anoxia/euxinia.

Influence of particle composition on thorium cycling along the U.S. GEOTRACES North Atlantic Section

NASA Astrophysics Data System (ADS)

Lerner, Paul; Marchal, Olivier; Lam, Phoebe

2017-04-01

Our current knowledge about the behaviour of particle-reactive substances in the ocean stems largely from measurements of thorium radio-isotopes (Th-228, Th-230, Th-234) on seawater samples. The oceanic Th database has increased dramatically over the recent years, thanks in particular to the GEOTRACES program, an international study of the marine biogeochemical cycles of trace elements and their isotopes. Here we present an analysis of data collected at several stations of the U.S. GEOTRACES North Atlantic section (section GA03). Data originating from eleven stations situated west and east of the Middle-Atlantic Ridge are analyzed. First, at each station, the rate parameters of a single-particle class model of Th and particle cycling in the ocean water column are estimated from a least-squares fit to an eclectic data set, including (i) measurements of Th-228, Th-230, Th-234 activities in different size fractions, (ii) measurements of particle concentration, and (iii) measurements, or observational estimates, of the activities of the radio-active parents Ra-228, U-234, and U-238. Among our most salient results is a significant decrease in the apparent rate constant of Th adsorption (k1) with depth, with maxima in the meso-pelagic zone (ca. 100 - 1000 m) and minima below, at most stations. Second, we explore whether our k1 estimates can be related to changes in particle composition, both along the water column and laterally along GA03. We apply (i) multiple linear regression to quantify the amount of variance in k1 that can be explained by linear regression against particle composition data, and (ii) relative importance analysis to determine the relative contribution of different particulate phases to the explained variance in k1. Finally, the implications of our results for the interpretation of field Th isotope data and for the description of particle scavenging in ocean-biogeochemistry models are clarified.

Determination of extremely low (236)U/(238)U isotope ratios in environmental samples by sector-field inductively coupled plasma mass spectrometry using high-efficiency sample introduction.

PubMed

Boulyga, Sergei F; Heumann, Klaus G

2006-01-01

A method by inductively coupled plasma mass spectrometry (ICP-MS) was developed which allows the measurement of (236)U at concentration ranges down to 3 x 10(-14)g g(-1) and extremely low (236)U/(238)U isotope ratios in soil samples of 10(-7). By using the high-efficiency solution introduction system APEX in connection with a sector-field ICP-MS a sensitivity of more than 5,000 counts fg(-1) uranium was achieved. The use of an aerosol desolvating unit reduced the formation rate of uranium hydride ions UH(+)/U(+) down to a level of 10(-6). An abundance sensitivity of 3 x 10(-7) was observed for (236)U/(238)U isotope ratio measurements at mass resolution 4000. The detection limit for (236)U and the lowest detectable (236)U/(238)U isotope ratio were improved by more than two orders of magnitude compared with corresponding values by alpha spectrometry. Determination of uranium in soil samples collected in the vicinity of Chernobyl nuclear power plant (NPP) resulted in that the (236)U/(238)U isotope ratio is a much more sensitive and accurate marker for environmental contamination by spent uranium in comparison to the (235)U/(238)U isotope ratio. The ICP-MS technique allowed for the first time detection of irradiated uranium in soil samples even at distances more than 200 km to the north of Chernobyl NPP (Mogilev region). The concentration of (236)U in the upper 0-10 cm soil layers varied from 2 x 10(-9)g g(-1) within radioactive spots close to the Chernobyl NPP to 3 x 10(-13)g g(-1) on a sampling site located by >200 km from Chernobyl.

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 wells show significantly lower δ238U values. High δ238U values in most of the wells located in the ore-zone may be attributed to the dissolution of the U ore enriched in 238U. The low δ238U values are generally observed in the wells with low U(VI) concentrations. Since U(VI) reduction fractionates 238U to the solid U(IV) phase, the depletion of 238U in the groundwater samples in the downgradient monitoring wells suggest U(VI) reduction by the downgradient sediments. The δ238U values in the groundwater samples conform to a Rayleigh distillation model with an isotopic fractionation factor α = 1.00013 × 0.00010. Future investigations include characterization of the U ore bearing sediments collected from boreholes in the ore body and downgradient of the ore body, measurement of the δ238U and δ82Se values in the ore and in remaining groundwater samples. The U(VI) reducing capacity and concomitant U isotopic fractionation factors for the sediments from downgradient boreholes will be determined from the batch incubation experiments and flow through column experiments.

Calorimetric low temperature detectors for low-energetic heavy ions and their application in accelerator mass spectrometry

NASA Astrophysics Data System (ADS)

Kraft-Bermuth, S.; Andrianov, V. A.; Bleile, A.; Echler, A.; Egelhof, P.; Kiseleva, A.; Kiselev, O.; Meier, H. J.; Meier, J. P.; Shrivastava, A.; Weber, M.; Golser, R.; Kutschera, W.; Priller, A.; Steier, P.; Vockenhuber, C.

2009-10-01

The energy-sensitive detection of heavy ions with calorimetric low temperature detectors was investigated in the energy range of E =0.1-1 MeV/amu, commonly used for accelerator mass spectrometry (AMS). The detectors used consist of sapphire absorbers and superconducting aluminum transition edge thermometers operated at T ˜1.5 K. They were irradiated with various ion beams (C13,A197u,U238) provided by the VERA tandem accelerator in Vienna, Austria. The relative energy resolution obtained was ΔE /E=(5-9)×10-3, even for the heaviest ions such as U238. In addition, no evidence for a pulse height defect was observed. This performance allowed for the first time to apply a calorimetric low temperature detector in an AMS experiment. The aim was to precisely determine the isotope ratio of U236/U238 for several samples of natural uranium, U236 being known as a sensitive monitor for neutron fluxes. Replacing a conventionally used detection system at VERA by the calorimetric detector enabled to substantially reduce background from neighboring isotopes and to increase the detection efficiency. Due to the high sensitivity achieved, a value of U236/U238=6.1×10-12 could be obtained, representing the smallest U236/U238 ratio measured at the time. In addition, we contributed to establishing an improved material standard of U236/U238, which can be used as a reference for future AMS measurements.

Multinucleon transfer in central collisions of 238U+238U

NASA Astrophysics Data System (ADS)

Ayik, S.; Yilmaz, B.; Yilmaz, O.; Umar, A. S.; Turan, G.

2017-08-01

Quantal diffusion mechanism of nucleon exchange is studied in the central collisions of 238U+238U in the framework of the stochastic mean-field (SMF) approach. For bombarding energies considered in this work, the dinuclear structure is maintained during the collision. Hence, it is possible to describe nucleon exchange as a diffusion process for mass and charge asymmetry. Quantal neutron and proton diffusion coefficients, including memory effects, are extracted from the SMF approach and the primary fragment distributions are calculated.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marinelli, R; Hamilton, T; Brown, T

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 Multimore » Collector Inductively Coupled Plasma Mass Spectrometry (MC ICP-MS), Accelerator Mass Spectrometry (AMS) and Alpha Spectrometry.« less

Image segmentation for uranium isotopic analysis by SIMS: Combined adaptive thresholding and marker controlled watershed approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Willingham, David G.; Naes, Benjamin E.; Heasler, Patrick G.

A novel approach to particle identification and particle isotope ratio determination has been developed for nuclear safeguard applications. This particle search approach combines an adaptive thresholding algorithm and marker-controlled watershed segmentation (MCWS) transform, which improves the secondary ion mass spectrometry (SIMS) isotopic analysis of uranium containing particle populations for nuclear safeguards applications. The Niblack assisted MCWS approach (a.k.a. SEEKER) developed for this work has improved the identification of isotopically unique uranium particles under conditions that have historically presented significant challenges for SIMS image data processing techniques. Particles obtained from five NIST uranium certified reference materials (CRM U129A, U015, U150, U500more » and U850) were successfully identified in regions of SIMS image data 1) where a high variability in image intensity existed, 2) where particles were touching or were in close proximity to one another and/or 3) where the magnitude of ion signal for a given region was count limited. Analysis of the isotopic distributions of uranium containing particles identified by SEEKER showed four distinct, accurately identified 235U enrichment distributions, corresponding to the NIST certified 235U/238U isotope ratios for CRM U129A/U015 (not statistically differentiated), U150, U500 and U850. Additionally, comparison of the minor uranium isotope (234U, 235U and 236U) atom percent values verified that, even in the absence of high precision isotope ratio measurements, SEEKER could be used to segment isotopically unique uranium particles from SIMS image data. Although demonstrated specifically for SIMS analysis of uranium containing particles for nuclear safeguards, SEEKER has application in addressing a broad set of image processing challenges.« less

Precise 238U(n,2n)237U reaction cross-section measurements using the activation facility at TUNL

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Bhike, M.; Tornow, W.

2014-09-01

Accurate neutron-induced 238U(n,2n)237U reaction data are required for many practical applications, especially in the field of nuclear energy, including advanced heavy water reactors, where 238U is used as the breeding material to regenerate the fissile material 239Pu. Precise (n,2n) cross-section measurements of 238U are underway at TUNL with mono-energetic neutrons in the 8.0 to 14.0 MeV energy range in steps of 0.25 MeV using the activation technique. After activation of the 0.5 inch diameter and 442 mg 238U foil, the activity of the 208 keV characteristic γ-line is tracked for 6 weeks with a high efficient HPGe clover detector to determine the initial activity needed for the cross-section determination. Results of the cross-section measurements, determined relative to 27Al and 197Au neutron activation monitor foils, and the comparison with theoretical models will be presented during the meeting.

Uranium 238U/235U isotope ratios as indicators of reduction: Results from an in situ biostimulation experiment at Rifle, Colorado, USA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bopp IV, C.J.; Lundstrom, C.C.; Johnson, T.M.

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 groundwatermore » 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)}.« less

Monte Carlo analyses of TRX slightly enriched uranium-H/sub 2/O critical experiments with ENDF/B-IV and related data sets (AWBA Development Program)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hardy, J. Jr.

1977-12-01

Four H/sub 2/O-moderated, slightly-enriched-uranium critical experiments were analyzed by Monte Carlo methods with ENDF/B-IV data. These were simple metal-rod lattices comprising Cross Section Evaluation Working Group thermal reactor benchmarks TRX-1 through TRX-4. Generally good agreement with experiment was obtained for calculated integral parameters: the epi-thermal/thermal ratio of U238 capture (rho/sup 28/) and of U235 fission (delta/sup 25/), the ratio of U238 capture to U235 fission (CR*), and the ratio of U238 fission to U235 fission (delta/sup 28/). Full-core Monte Carlo calculations for two lattices showed good agreement with cell Monte Carlo-plus-multigroup P/sub l/ leakage corrections. Newly measured parameters for themore » low energy resonances of U238 significantly improved rho/sup 28/. In comparison with other CSEWG analyses, the strong correlation between K/sub eff/ and rho/sup 28/ suggests that U238 resonance capture is the major problem encountered in analyzing these lattices.« less

Combined Th/U, Pa/U and Ra/Th dating of fossil reef corals

NASA Astrophysics Data System (ADS)

Obert, J. C.; Scholz, D.; Lippold, J.; Felis, T.; Jochum, K. P.; Andreae, M. O.

2016-12-01

Fossil reef corals are often subject to post-depositional open-system behaviour, which is a major problem for accurate absolute dating. The commonly used 230Th/U-system can be disturbed by diagenetic alteration resulting in wrong apparent 230Th/U-ages. Since fossil reef corals are important palaeoenvironmental archives, precise absolute dating is essential for sea-level reconstruction and high-resolution climate reconstruction. We have developed a method for combined preparation and analysis of fossil reef corals by the 230Th/U-, 231Pa/U- and 226Ra/230Th-methods. Inconsistencies between ages determined by the different methods provide a means to identify diagenetically altered corals. In addition, the comparison of the 230Th/U and 231Pa/U data on concordia diagrams reveals further information about the alteration processes. (226Ra/230Th) and (226Ra/U) ratios in particular provide information about the more recent past (last 10 to approx. 50 ka) of the coral's diagenetic history. We compare these data with quantitative modelling of various diagenetic scenarios in order to identify the potential open-system processes. Here we present new data on the combined application of the three isotope systems to fossil Last Interglacial corals from the Gulf of Aqaba, northern Red Sea. Previous studies have shown that these corals were subject to substantial open-system behaviour, documented by very high initial (234U/238U) activity ratios. The process that was proposed to explain the activity ratios of these corals is U gain with subsequent U loss after a specific amount of time. The amount of U loss is assumed to be proportional to the amount of U previously gained. The application of our new method aims to test whether this diagenetic scenario can be verified.

Initial Eccentricity in Deformed 197Au+197Au and 238U+238U Collisions at RHIC

DOE Office of Scientific and Technical Information (OSTI.GOV)

Filip, Peter; Lednicky, Richard; Masui, Hiroshi

2010-07-07

Initial eccentricity and eccentricity fluctuations of the interaction volume created in relativistic collisions of deformed {sup 197}Au and {sup 238}U nuclei are studied using optical and Monte-Carlo (MC) Glauber simulations. It is found that the non-sphericity noticeably influences the average eccentricity in central collisions and eccentricity fluctuations are enhanced due to deformation. Quantitative results are obtained for Au+Au and U+U collisions at energy {radical}s{sub NN} = 200 GeV.

Uranium activity ratio in water and fish from pit lakes in Kurday, Kazakhstan and Taboshar, Tajikistan.

PubMed

Strømman, G; Rosseland, B O; Skipperud, L; Burkitbaev, L M; Uralbekov, B; Heier, L S; Salbu, B

2013-09-01

Kurday in Kazhakstan and Taboshar in Tajikistan were U mining sites operated during the 1950s and 1960s as part of the USSR nuclear weapon program. Today, they represent sources of potential U contamination of the environment. Within both mining sites, open pits from which U ore was extracted have been filled with water due to ground water inflow and precipitation. These artificial pit lakes contain fish consumed occasionally by the local people, and wild and domestic animals are using the water for drinking purposes. To assess the potential impact from U in these pit lakes, field work was performed in 2006 in Kurday and 2006 and 2008 in Taboshar. Results show that the U concentration in the lake waters were relatively high, about 1 mg/L in Kurday Pit Lake and about 3 mg/L in Taboshar Pit Lake. The influence of U-bearing materials on the lakes and downstream waters were investigated by measuring the U concentration and the (234)U/(238)U activity ratios. In both Kurday and Taboshar, the ratios increased distinctively from about 1 at the pit lakes to >1.5 far downstream the lakes. The concentrations of (238)U in gill, liver, muscle and bones in fish from the pit lakes were much higher than in the reference fish. Peak concentration of U was seen in bones (13 mg/kg w.w.), kidney (9.1 mg/kg w.w.) and gills (8.9 mg/kg w.w.) from Cyprinus auratus caught in the Taboshar Pit Lake. Bioconcentration factors (BCF) calculated for organs from fish caught in the Taboshar Pit Lake, with the same tendency seen in the Kurday Pit Lake, showed that U accumulates most in bone (BCF = 4.8 L/kg w.w.), gills (BCF = 3.6 L/kg w.w.), kidney (BCF = 3.6 L/kg w.w.), and liver (BCF = 2.5 L/kg w.w.), while least was accumulated in the muscle (BCF = 0.12 L/kg w.w.). Copyright © 2012 Elsevier Ltd. All rights reserved.

Adiabatic and coupled channels calculations for near barrier fusion of 16O +238U using realistic nucleon-nucleon interaction

NASA Astrophysics Data System (ADS)

Ismail, M.; Seif, W. M.; Botros, M. M.

2016-04-01

We investigate the fusion cross-section and the fusion barrier distribution of 16O +238U at near- and sub-barrier energies. We use an interaction potential generated by the semi-microscopic double folding model-based on density dependent (DD) form of the realistic Michigan-three-Yukawa (M3Y) Reid nucleon-nucleon (NN) interaction. We studied the role of both the static and dynamic deformations of the target nucleus on the fusion process. Rotational and vibrational degrees of freedom of 238U-nucleus are considered. We found that the deformation and the octupole vibrations in 238U enhance its sub-barrier fusion cross-section. The signature of the the octupole vibrational modes of 238U appears clearly in its fusion barrier distribution profile.

Behaviors of 323Th, 238U, 228Ra and 226Ra on combustion of crude oil terminal sludge.

PubMed

Puad, H A Mohamad; Noor, M Y Muhd

2004-01-01

Crude oil terminal sludge contains technologically enhanced naturally occurring radionuclides such as (232)Th, (238)U, (228)Ra and (226)Ra, thus cannot be disposed of freely without proper control. The current method of disposal, such as land farming and storing in plastic drums is not recommended because it will have a long-term impact on the environment. Due to its organic nature, there is a move to treat this sludge by thermal methods such as incineration. This study has been carried out to determine the behaviors of (232)Th, (238)U, (228)Ra and (226)Ra present in the sludge during combustion at a certain temperature and time. The percentage of volatilization was found to vary between 2% and 70%, (238)U was the most volatile in comparison with (232)Th, (228)Ra and (226)Ra. (238)U is found to be significantly volatilized above 500 degrees C, and might reach maximum volatilization at above 700 degrees C. A mathematical model was developed to predict the percentage of volatilization of (232)Th, (238)U, (228)Ra and (226)Ra contained in the sludge. With this known percentage of volatilization, the concentration of (232)Th, (238)U, (228)Ra and (226)Ra present in the bottom and filter ashes can be calculated.

Th-230 - U-238 series disequilibrium of the Olkaria rhyolites Gregory Rift Valley, Kenya: Petrogenesis

NASA Technical Reports Server (NTRS)

Black, S.; Macdonald, R.; Kelly, M.

1993-01-01

Positive correlations of (U-238/Th-230) versus Th show the rhyolites to be products of partial melting. Positive correlations of U and Cl and U and F show that the U enrichment in the rhyolites is associated with the halogen contents which may be related to the minor phenocryst phase fractionation. Instantaneous Th/U ratios exceed time integrated Th/U ratios providing further evidence of the hydrous nature of the Olkaria rhyolite source. Excess (U-238/Th-230) in the subduction related rocks has been associated to the preferential incorporation of uranium in slab derived fluids, but no evaluation of the size of this flux has been made. The majority of the Naivasha samples show a (U-238/Th-230) less than 1 and plot close to the subduction related samples indicating the Naivasha rhyolites may also have been influenced by fluids during their formation. In general samples with high (U-238/Th-230) ratios reflecting recent enrichment of uranium relative to thorium have high thorium contents, thereby the high (U-238/Th-230) ratios are restricted to the most incompatible element enriched magmas and, hence, are a good indication that the rhyolites were formed by partial melting. If a fluid phase had some influence on the formation of the rhyolites then the uranium and thorium may have some correlation with F and Cl contents which can be mirrored by the peralkalinity. Plots of uranium against F and Cl contents are shown. The positive correlation indicates that the uranium enrichments are associated with the halogen contents. There seems to be a greater correlation for U against Cl than F indicating that the U may be transported preferentially as Cl complexes.

Late summer particulate organic carbon export and twilight zone remineralisation in the Atlantic sector of the Southern Ocean

NASA Astrophysics Data System (ADS)

Planchon, F.; Cavagna, A.-J.; Cardinal, D.; André, L.; Dehairs, F.

2012-03-01

During the Bonus-GoodHope (BGH) expedition (Jan-Mar 2008) we studied the water column distribution of total 234Th and biogenic particulate Ba (Baxs) in the Atlantic sector of the Southern Ocean. The objective was to assess the export flux of particulate organic carbon (POC) from the surface to the mesopelagic twilight zone along a section between the Cape Basin and Weddell Gyre. Export production of POC was estimated from steady state and non steady state export fluxes of 234Th which were converted into POC fluxes, using the POC/234Th ratio of large (>53 μm) suspended particles, collected via in-situ pumps. Deficits in 234Th activities were observed at all stations from the surface to the bottom of the mixed-layer. 234Th export fluxes from the upper 100 m ranged from 496 ± 57 dpm m-2 d-1 to 1195 ± 120 dpm m-2 d-1 for the steady state model and from 149 ± 18 dpm m-2 d-1 to 1217 ± 146 dpm m-2 d-1 for the non steady state model calculated for a time window of 15 to 22 days preceding the timing of the present cruise. The POC/234Thp ratio of large, potentially sinking particles (>53 μm), was observed to increase with latitude, from 1.9 ± 0.2 μmol dpm-1 and 1.7 ± 0.3 μmol dpm-1 in the Subtropical Zone (STZ) and Subantarctic Zone (SAZ), respectively, to 3.0 ± 0.2 μmol dpm-1 in the Polar Front Zone (PFZ), 4.8 ± 1.9 μmol dpm-1 at the Southern Antarctic Circumpolar Current Front (SACCF) to 4.1 ± 1.7 μmol dpm-1 in the northern Weddell Gyre, in line with an increasing contribution of larger cell diatoms. Steady state and non steady state POC export from the upper 100 m ranged from 0.9 ± 0.2 mmolC m-2 d-1 to 5.1 ± 2.1 mmolC m-2 d-1 and from 0.3 ± 0.0 mmolC m-2 d-1 to 4.9 ± 3.2 mmolC m-2 d-1, respectively. From the SAZ to the SACCF, non steady state POC export production represented only 15 to 54 % of the steady state POC flux, suggesting that the intensity of export had decreased over time partly due to the fact that regenerated-production based communities of small-sized phytoplankton became predominant. In contrast, for the HNLC area south of the SACCF, we found an excellent agreement between the two modeling approaches indicating that surface POC export remained rather constant there. Estimated POC export represented between 6 to 54 % of the potential export as represented by new production, indicating that export efficiency was particularly low throughout the studied area, except close to the SACCF. Below the export layer, in the mesopelagic zone, 234Th activities generally reached equilibrium with 238U, but sometimes were in large excess relative to 238U (234Th/238U ratio>1.1), reflecting intense remineralisation/disaggregation of 234Th-bearing particles. The accumulation of excess 234Th in the 100-600 m depth interval ranged from 458 ± 55 dpm m-2 d-1 to 3068 ± 368 dpm m-2 d-1. Using POC to 234Th ratio of sinking particles, we converted this 234Th flux into a POC remineralisation flux, which ranged between 0.9 to 9.2 mmolC m-2 d-1. Mesopelagic remineralisation was also evidenced by Baxs inventories which are related to bacterial degradation of sinking material and offer a means to quantify the flux of respired C. Highest biogenic particulate Ba (Baxs) contents were generally observed in the 200-400 m depth interval with values reaching up to >1000 pM in the northern PFZ. Depth weighted average mesopelagic Baxs (meso-Baxs) was high in the PFZ and low in the northernmost (STZ-SAZ) and the southernmost (SACCF-AZ-WG) parts of the BGH section; conversion into respired C flux yielded a range of -0.23 to 6.4 mmolC m-2 d-1. Excluding two outliers, we found a significant positive correlation for mesopelagic waters between POC remineralisation estimated from meso-Baxs and from 234Th excess (R2 = 0.73). Our results indicate that POC export production in this area of the Southern Ocean was strongly attenuated in the mesopelagic waters due to remineralisation, a process which thus appears to strongly impact on longer term bathypelagic zone sequestration of POC.

Study of Heavy-ion Induced Fission for Heavy Element Synthesis

NASA Astrophysics Data System (ADS)

Nishio, K.; Ikezoe, H.; Hofmann, S.; Ackermann, D.; Aritomo, Y.; Comas, V. F.; Düllmann, Ch. E.; Heinz, S.; Heredia, J. A.; Heßberger, F. P.; Hirose, K.; Khuyagbaatar, J.; Kindler, B.; Kojouharov, I.; Lommel, B.; Makii, M.; Mann, R.; Mitsuoka, S.; Nishinaka, I.; Ohtsuki, T.; Saro, S.; Schädel, M.; Popeko, A. G.; Türler, A.; Wakabayashi, Y.; Watanabe, Y.; Yakushev, A.; Yeremin, A.

2014-05-01

Fission fragment mass distributions were measured in heavy-ion induced fission of 238U. The mass distributions changed drastically with incident energy. The results are explained by a change of the ratio between fusion and quasifission with nuclear orientation. A calculation based on a fluctuation dissipation model reproduced the mass distributions and their incident energy dependence. Fusion probability was determined in the analysis. Evaporation residue cross sections were calculated with a statistical model for the reactions of 30Si+238U and 34S+238U using the obtained fusion probability in the entrance channel. The results agree with the measured cross sections of 263,264Sg and 267,268Hs, produced by 30Si+238U and 34S+238U, respectively. It is also suggested that sub-barrier energies can be used for heavy element synthesis.

Formation of stable uranium(VI) colloidal nanoparticles in conditions relevant to radioactive waste disposal.

PubMed

Bots, Pieter; Morris, Katherine; Hibberd, Rosemary; Law, Gareth T W; Mosselmans, J Frederick W; Brown, Andy P; Doutch, James; Smith, Andrew J; Shaw, Samuel

2014-12-09

The favored pathway for disposal of higher activity radioactive wastes is via deep geological disposal. Many geological disposal facility designs include cement in their engineering design. Over the long term, interaction of groundwater with the cement and waste will form a plume of a hyperalkaline leachate (pH 10-13), and the behavior of radionuclides needs to be constrained under these extreme conditions to minimize the environmental hazard from the wastes. For uranium, a key component of many radioactive wastes, thermodynamic modeling predicts that, at high pH, U(VI) solubility will be very low (nM or lower) and controlled by equilibrium with solid phase alkali and alkaline-earth uranates. However, the formation of U(VI) colloids could potentially enhance the mobility of U(VI) under these conditions, and characterizing the potential for formation and medium-term stability of U(VI) colloids is important in underpinning our understanding of U behavior in waste disposal. Reflecting this, we applied conventional geochemical and microscopy techniques combined with synchrotron based in situ and ex situ X-ray techniques (small-angle X-ray scattering and X-ray adsorption spectroscopy (XAS)) to characterize colloidal U(VI) nanoparticles in a synthetic cement leachate (pH > 13) containing 4.2-252 μM U(VI). The results show that in cement leachates with 42 μM U(VI), colloids formed within hours and remained stable for several years. The colloids consisted of 1.5-1.8 nm nanoparticles with a proportion forming 20-60 nm aggregates. Using XAS and electron microscopy, we were able to determine that the colloidal nanoparticles had a clarkeite (sodium-uranate)-type crystallographic structure. The presented results have clear and hitherto unrecognized implications for the mobility of U(VI) in cementitious environments, in particular those associated with the geological disposal of nuclear waste.

Uranium (238U)-induced ROS and cell cycle perturbations, antioxidant responses and erythrocyte nuclear abnormalities in the freshwater iridescent shark fish Pangasius sutchi.

PubMed

Annamalai, Sathesh Kumar; Arunachalam, Kantha Deivi

2017-05-01

The strategic plan of this study is to analyze any possible radiological impact on aquatic organisms from forthcoming uranium mining facilities around the Nagarjuna Sagar Dam in the future. The predominantly consumed and dominant fish species Pangasius sutchi, which is available year-round at Nagarjuna Sagar Dam, was selected for the study. To comprehend the outcome and to understand the mode of action of 238 U, the fish species Pangasius sutchi was exposed to ¼ and ½ of the LC 50 doses of waterborne 238 U in a static system in duplicate for 21 days. Blood and organs, including the gills, liver, brain and muscles, were collected at different time periods-0h, 24h, 48h, 72h, 96h, 7, days 14days and 21 days-using ICP-MS to determine the toxic effects of uranium and the accumulation of 238 U concentrations. The bioaccumulation of 238 U in P. sutchi tissues was dependent on exposure time and concentration. The accumulation of uranium was, in order of magnitude, measured as gills>liver>brain>tissue, with the highest accumulation in the gills. It was observed that exposure to 238 U significantly reduced antioxidant enzymes such as superoxide dismutase, catalase, and lipid peroxidase. The analysis of DNA fragmentation by comet assay and cell viability by flow cytometry was performed at different time intervals. DNA histograms by flow cytometry analysis revealed an increase in the G2/M phase and the S phase. The long-term 238 U exposure studies in fish showed increasing micronucleus frequencies in erythrocytes with greater exposure time. The higher the concentration of 238 U is, the greater is the effect observed, suggesting a close relationship between accumulation and toxicity. A possible ROS-mediated 238 U toxicity mechanism and antioxidant responses have been proposed. Copyright © 2017 Elsevier B.V. All rights reserved.

Control of the U and Th behaviour in forest soils

NASA Astrophysics Data System (ADS)

Rihs, Sophie; Gontier, Adrien; Chabaux, François; Pelt, Eric; Turpault, Marie-Pierre

2015-04-01

U- and Th-series disequilibria and U, Th, Fe and Al speciation, were measured in several soil profiles from the experimental forest site of Breuil (Morvan, France) in order to address the impact of the vegetation on U and Th nuclides behaviour in soils. Thirty-five years after an experimental clear-felling of the native forest, the soil developed under two replacing mono-specific plantations (Oak and Douglas fir) were therefore compared to the undisturbed native forest soil. The analogous physical and chemical properties of these soils before the replacement were formerly demonstrated. Our results suggest that a shift in the Iron distribution seems to occur under the stand replaced by Oaks, with a significant replacement of Fe-bearing silicates by well crystallized Fe oxides. In contrast, such evolution was not demonstrated in the soils under Douglas fir. The concurrent loss of U and Th from the soils under Oak was tentatively related to the dissolution of Fe-bearing minerals. A mass balance calculation demonstrates that the observed increase in U oxalate-extracted fractions can quantitatively be explained through the entire profiles by a mere dissolution of up to 20% of U-Fe-bearing silicated minerals, without significant re-adsorption onto the amorphous Fe-Al oxides for U. Beside this primary release from Fe-bearing silicate minerals, the mobility of U and Th seems more likely controlled by Al phases rather than Fe oxides in surface layers during further pedogenic processes. Indeed, some of the U- and Th series disequilibria seem to be strongly related to Al dynamic in these layers. This relationship can be seen in the native forest profiles as well as in the replaced profiles, suggesting that this feature is not linked to the cover change. The redistribution of U and Th isotopes through these pedogenic processes therefore rule out the use of U-series for weathering rate determination in shallowest soils layers. In contrast, below 25 cm, the release of U and Th as well as the change of their distribution among the soil phases does not affect U- and Th series disequilibria. The activity ratios measured in oxalate leachates and the residues allow to demonstrate that the dissolution of a U-bearing silicate mineral and the consequent release of up to 20% of U would shift the (234U/238U) and (230Th/234U) ratios by less than 2%. These results therefore reveal that, after 35 years, no significant impact of the cover change on U-series disequilibria was recorded in the main part of the soil profiles, which, at this stage, justify the use of these nuclides as chronometers for weathering determination.

An alternative procedure for uranium analysis in drinking water using AQUALIX columns: application to varied French bottled waters.

PubMed

Bouvier-Capely, C; Bonthonneau, J P; Dadache, E; Rebière, F

2014-01-01

The general population is chronically exposed to uranium ((234)U, (235)U, and (238)U) and polonium ((210)Po) mainly through day-to-day food and beverage intake. The measurement of these naturally-occurring radionuclides in drinking water is important to assess their health impact. In this work the applicability of calix[6]arene-derivatives columns for uranium analysis in drinking water was investigated. A simple and effective method was proposed on a specific column called AQUALIX, for the separation and preconcentration of U from drinking water. This procedure is suitable for routine analysis and the analysis time is considerably shortened (around 4h) by combining the separation on AQUALIX with fast ICP-MS measurement. This new method was tested on different French bottled waters (still mineral water, sparkling mineral water, and spring water). Then, the case of simultaneous presence of uranium and polonium in water was considered due to interferences in alpha spectrometry measurement. A protocol was proposed using a first usual step of spontaneous deposition of polonium on silver disc in order to separate Po, followed by the uranium extraction on AQUALIX column before alpha spectrometry counting. © 2013 Published by Elsevier B.V.

First application of calorimetric low-temperature detectors in accelerator mass spectrometry

NASA Astrophysics Data System (ADS)

Kraft, S.; Andrianov, V.; Bleile, A.; Egelhof, P.; Golser, R.; Kiseleva, A.; Kiselev, O.; Kutschera, W.; Meier, J. P.; Priller, A.; Shrivastava, A.; Steier, P.; Vockenhuber, C.

2004-03-01

For the first time, calorimetric low-temperature detectors were applied in accelerator mass spectrometry, a well-known method for determination of very small isotope ratios with high sensitivity. The aim of the experiment was to determine with high accuracy the isotope ratio of 236U/238U for several samples of natural uranium, 236U being known as a sensitive monitor for neutron flux. Measurements were performed at the VERA tandem accelerator at Vienna, Austria. The detectors consist of sapphire absorbers and superconducting transition edge thermometers operated at T≈ 1.5 K. The relative energy resolution obtained for 17.39 MeV 238U is ΔE/E=4-9×10-3, depending on the experimental conditions. This performance enabled to substantially reduce background from neighbouring isotopes and to increase the detection efficiency. Due to the high sensitivity achieved, a value of 236U/238U=6.5×10-12 could be obtained, representing the smallest 236U/238U ratio measured until now.

Prospects of heavy and superheavy element production via inelastic nucleus-nucleus collisions - from 238U+238U to18O+254Es

NASA Astrophysics Data System (ADS)

Schädel, Matthias

2016-12-01

Multi-nucleon transfer reactions, frequently termed deep-inelastic, between heavy-ion projectiles and actinide targets provide prospects to synthesize unknown isotopes of heavy actinides and superheavy elements with neutron numbers beyond present limits. The 238U on 238U reaction, which revealed essential aspects of those nuclear reactions leading to surviving heavy nuclides, mainly produced in 3n and 4n evaporation channels, is discussed in detail. Positions and widths of isotope distributions are compared. It is shown, as a general rule, that cross sections peak at irradiation energies about 10% above the Coulomb barrier. Heavy target nuclei are essential for maximizing cross sections. Experimental results from the 238U on 248Cm reaction, including empirical extrapolations, are compared with theoretical model calculations predicting relatively high cross sections for neutron-rich nuclei. Experiments to test the validity of such predictions are proposed. Comparisons between rather symmetric heavy-ion reactions like 238U on 248Cm (or heavier targets up to 254Es) with very asymmetric ones like 18O on 254Es reveal that the ones with 238U as a projectile have the highest potential in the superheavy element region while the latter ones can be advantageous for the synthesis of heavy actinide isotopes. Concepts for highly efficient recoil separators designed for transfer products are presented.

A search for isotopic anomalies in uranium. [in chondritic meteorites and terrestrial basalt

NASA Technical Reports Server (NTRS)

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

1980-01-01

The U-238/U-235 ratios for nine bulk chondritic meteorites and a terrestrial basalt were measured. The total range in U-238/U-235 determined for both total meteorites and for acid leaches was from 137.2 terrestrial U. The typical errors in a single determination are plus or minus 6 per thousand (2 sigma m) for a 2 ng U sample from a chondrite. Taking the extreme values of delta U-235 for each measurement the maximum amount of excess U-235 that can be allowed to be present ranges from 200 million to 2 billion atoms per gram of bulk meteorite. These results do not support the claims of variations in U-238/U-235 at the percentage levels or number of excess U-235 atoms in some of the same meteorites as reported by several other previous workers.

^2^3^8U/^2^3^5U Ratios of Anagrams: Angrites and Granites

NASA Astrophysics Data System (ADS)

Tissot, F. L. H.; Dauphas, N.

2012-03-01

We report ^2^3^8U/^2^3^5U ratios of five angrites and give the corresponding Pb-Pb ages of D'Orbigny and Angra Dos Reis. The U-isotopic composition of terrestrial granites (I, S, and A types) is also assessed to determine the influence of the protolith.

Internal dose assessment of 238U contaminated soils based on in-vitro gastrointestinal protocol

NASA Astrophysics Data System (ADS)

Perama, Yasmin Mohd Idris; Rashid, Nur Shahidah Abdul; Majid, Amran Ab.; Siong, Khoo Kok

2017-01-01

Human exposure to natural radioactive uranium has been a great interest as more industrial rapidly growing contributes to radiation risks. The aim of this case study was to determine the internal dose in humans incorporated with ingestion of 238U contaminated soils. A gastrointestinal analogue test was employed to simulate the human digestive tract. In-vitro approach via German DIN 19738 model was developed in order to estimate the internal exposure of 238U due to ingestion of different types of soils. Synthetic gastrointestinal fluids assay via in-vitro method were produced to determine the concentration of 238U in various soils using ICP-MS. Based on the results, concentration of 238U in BRIS, laterite, peat and alluvium soils were in ranged between (0.0061 ± 0.0057 - 0.0488 ± 0.0148) ppm and (0.0005 ± 0.0004 - 0.0046 ± 0.0007) ppm in gastric and gastrointestinal phase respectively. Types of soil compositions and pH medium were some of the factors that influence mobilization and solubility of 238U contaminanted soil into the digestive juices that resembles human gastrointestinal tract. For the purpose of internal dose assessment, the committed efective dose from 238U intake in soils ranged between 1.237 × 10-11 - 9.8993 × 10-11 Sv y-1 for gastric phase and 1.0184 × 10-12 - 9.3294 × 10-12 Sv y-1 for gastric-intestinal phase. The internal dose measurements from this study were much lower from the recommended values. Hence, ingestion of 238U contaminated soils would not be expected to pose major health risk to humans.

Fusion-fission Study at JAEA for Heavy-element Synthesis

NASA Astrophysics Data System (ADS)

Nishio, K.

Fission fragment mass distributions were measured in the heavy-ion induced fission using 238U target nucleus. The mass distribu- tions changed drastically with incident energy. The results are explained by a change of the ratio between fusion and qasifission with nuclear orientation. A calculation based on a fluctuation dissipation model reproduced the mass distributions and their inci- dent energy dependence. Fusion probability was determined in the analysis. Evaporation residue cross sections were calculated with a statistical model in the reactions of 30Si+238U and 34S+238U using the obtained fusion probability in the entrance channel. The results agree with the measured cross sections of 263,264Sg and 267,268Hs, produced by 30Si+238U and 34S+238U, respectively. It is also suggested that the sub-barrier energies can be used for heavy element synthesis.

In-beam fissio study at JAEA for heavy element synthesis

NASA Astrophysics Data System (ADS)

Nishio, K.; Ikezoe, H.; Hofmann, S.; Ackermann, D.; Aritomo, Y.; Comas, V. F.; Düllmann, Ch. E.; Heinz, S.; Heredia, J. A.; Heßberger, F. P.; Hirose, K.; Khuyagbaatar, J.; Kindler, B.; Kojouharov, I.; Lommel, B.; Makii, M.; Mann, R.; Mitsuoka, S.; Nishinaka, I.; Ohtsuki, T.; Saro, S.; Schädel, M.; Popeko, A. G.; Türler, A.; Wakabayashi, Y.; Watanabe, Y.; Yakushev, A.; Yeremin, A.

2013-04-01

Fission fragment mass distributions were measured in the heavy-ion induced fission using 238U target nucleus. The mass distributions changed drastically with incident energy. The results are explained by a change of the ratio between fusion and qasifission with nuclear orientation. A calculation based on a fluctuation dissipation model reproduced the mass distributions and their incident energy dependence. Fusion probability was determined in the analysis. Evaporation residue cross sections were calculated with a statistical model in the reactions of 30Si+238U and 34S+238U using the obtained fusion probability in the entrance channel. The results agree with the measured cross sections of 263,264Sg and 267,268Hs, produced by 30Si+238U and 34S+238U, respectively. It is also suggested that the sub-barrier energies can be used for heavy element synthesis.

Generation of 238U Covariance Matrices by Using the Integral Data Assimilation Technique of the CONRAD Code

NASA Astrophysics Data System (ADS)

Privas, E.; Archier, P.; Bernard, D.; De Saint Jean, C.; Destouche, C.; Leconte, P.; Noguère, G.; Peneliau, Y.; Capote, R.

2016-02-01

A new IAEA Coordinated Research Project (CRP) aims to test, validate and improve the IRDF library. Among the isotopes of interest, the modelisation of the 238U capture and fission cross sections represents a challenging task. A new description of the 238U neutrons induced reactions in the fast energy range is within progress in the frame of an IAEA evaluation consortium. The Nuclear Data group of Cadarache participates in this effort utilizing the 238U spectral indices measurements and Post Irradiated Experiments (PIE) carried out in the fast reactors MASURCA (CEA Cadarache) and PHENIX (CEA Marcoule). Such a collection of experimental results provides reliable integral information on the (n,γ) and (n,f) cross sections. This paper presents the Integral Data Assimilation (IDA) technique of the CONRAD code used to propagate the uncertainties of the integral data on the 238U cross sections of interest for dosimetry applications.

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 (1.29% organic carbon) below well-oxygenated bottom waters (-0.22 permil, n=1) are identical. The δ238U value matches previously reported values for suboxic sediments from the Peru margin [3], but is lighter than organic rich sediments from the Black Sea [3], where the bottom waters are strongly euxinic. The consistency in δ238U vaues between previously investigated suboxic sediment samples [3] and our two sediment samples indicates that the magnitude of the U isotopic fractionation is identical between seawater and sediments deposited under a range of bottom water oxygen conditions from oxygenated to anoxic. However, differences between the U isotope compositions in Saanich Inlet and those from the Black Sea remain to be explained, if U isotope fractionation is be used as a quantitative proxy for paleoredox in ancient oceans. [1] Schauble (2007) GCA 71, 2170- 2189. [2] Stirling et al. (2007) EPSL 264, 208-225. [3] Weyer et al. (2007) GCA 72, 345-399.

230Th/U dating of a late Pleistocene alluvial fan along the southern San Andreas fault

USGS Publications Warehouse

Fletcher, Kathryn E.K.; Sharp, Warren D.; Kendrick, Katherine J.; Behr, Whitney M.; Hudnut, Kenneth W.; Hanks, Thomas C.

2010-01-01

U-series dating of pedogenic carbonate-clast coatings provides a reliable, precise minimum age of 45.1 ± 0.6 ka (2σ) for the T2 geomorphic surface of the Biskra Palms alluvial fan, Coachella Valley, California. Concordant ages for multiple subsamples from individual carbonate coatings provide evidence that the 238U-234U-230Th system has remained closed since carbonate formation. The U-series minimum age is used to assess previously published 10Be exposure ages of cobbles and boulders. All but one cobble age and some boulder 10Be ages are younger than the U-series minimum age, indicating that surface cobbles and some boulders were partially shielded after deposition of the fan and have been subsequently exhumed by erosion of fine-grained matrix to expose them on the present fan surface. A comparison of U-series and 10Be ages indicates that the interval between final alluvial deposition on the T2 fan surface and accumulation of dateable carbonate is not well resolved at Biskra Palms; however, the “time lag” inherent to dating via U-series on pedogenic carbonate can be no larger than ∼10 k.y., the uncertainty of the 10Be-derived age of the T2 fan surface. Dating of the T2 fan surface via U-series on pedogenic carbonate (minimum age, 45.1 ± 0.6 ka) and 10Be on boulder-top samples using forward modeling (preferred age, 50 ± 5 ka) provides broadly consistent constraints on the age of the fan surface and helps to elucidate its postdepositional development.

230Th/U dating of a late pleistocene alluvial fan along the southern san andreas fault

USGS Publications Warehouse

Fletcher, K.E.K.; Sharp, W.D.; Kendrick, K.J.; Behr, W.M.; Hudnut, K.W.; Hanks, T.C.

2010-01-01

U-series dating of pedogenic carbonate-clast coatings provides a reliable, precise minimum age of 45.1 ?? 0.6 ka (2??) for the T2 geomorphic surface of the Biskra Palms alluvial fan, Coachella Valley, California. Concordant ages for multiple subsamples from individual carbonate coatings provide evidence that the 238U-234U-230Th system has remained closed since carbonate formation. The U-series minimum age is used to assess previously published 10Be exposure ages of cobbles and boulders. All but one cobble age and some boulder 10Be ages are younger than the U-series minimum age, indicating that surface cobbles and some boulders were partially shielded after deposition of the fan and have been subsequently exhumed by erosion of fine-grained matrix to expose them on the present fan surface. A comparison of U-series and 10Be ages indicates that the interval between final alluvial deposition on the T2 fan surface and accumulation of dateable carbonate is not well resolved at Biskra Palms; however, the "time lag" inherent to dating via U-series on pedogenic carbonate can be no larger than ~10 k.y., the uncertainty of the 10Be-derived age of the T2 fan surface. Dating of the T2 fan surface via U-series on pedogenic carbonate (minimum age, 45.1 ?? 0.6 ka) and 10Be on boulder-top samples using forward modeling (preferred age, 50 ?? 5 ka) provides broadly consistent constraints on the age of the fan surface and helps to elucidate its postdepositional development. ?? 2010 Geological Society of America.

Initial eccentricity in deformed {sup 197}Au+{sup 197}Au and {sup 238}U+{sup 238}U collisions at {radical}(s{sub NN})=200 GeV at the BNL Relativistic Heavy Ion Collider

DOE Office of Scientific and Technical Information (OSTI.GOV)

Filip, Peter; Lednicky, Richard; Masui, Hiroshi

2009-11-15

Initial eccentricity and eccentricity fluctuations of the interaction volume created in relativistic collisions of deformed {sup 197}Au and {sup 238}U nuclei are studied using optical and Monte Carlo (MC) Glauber simulations. It is found that the nonsphericity noticeably influences the average eccentricity in central collisions, and eccentricity fluctuations are enhanced from deformation. Quantitative results are obtained for Au+Au and U+U collisions at energy {radical}(s{sub NN})=200 GeV.

The ability of Helianthus annuus L. and Brassica juncea to uptake and translocate natural uranium and 226Ra under different milieu conditions.

PubMed

Vera Tomé, F; Blanco Rodríguez, P; Lozano, J C

2009-01-01

Seedlings of Helianthus annuus L. (HA) and Brassica juncea (BJ) were used to test the effect of the pH, the presence of phosphates, and the addition of ethylene-diamine-tetraacetic acid (EDTA) or citrate on the uptake and the translocation of uranium isotopes ((238)U, (235)U, and (234)U) and (226)Ra. The results indicated that the presence of phosphates generally reduces the uptake and transfer of uranium from the roots to the shoots of HA. In the case of BJ, while phosphate enhanced the retention of uranium by roots, the translocation was poorer. Likewise, for (226)Ra, the best translocation was in the absence of phosphates for both species. The addition of citrate increased the translocation of uranium for both species, but had no clear effect on the transfer of (226)Ra. The effect of EDTA was much more moderate both for uranium and for (226)Ra, and for both plant species. Only noticeable was a slightly better uptake of (226)Ra by BJ at neutral pH, although the translocation was lower.

Evaluation of the use of reverse osmosis to eliminate natural radionuclides from water samples.

PubMed

Nieto, Antonio; Palomo, Marta; Ruana, Josep; Peñalver, Alejandra; Aguilar, Carme; Borrull, Francesc

2013-12-01

The objective of drinking water treatment plants (DWTP) is to supply the population with tap water that is in optimal condition and in compliance with water quality regulations. In the DWTP of L'Ampolla (Tarragona, Spain), slightly high values of gross alpha activity and the amount of salts in the raw water have been observed. Conventional treatment has reduced these levels only minimally. This study tested a tertiary treatment based on reverse osmosis is tested in an industrial pilot plant (240 m3/day) The efficiency of this pilot plant to reduce the gross alpha and beta activities and the activity of some individual radioisotopes (U(238), U(234), U(235) and Ra(226)) was tested. Results showed that the elimination of alpha emitters was greater than 90%, whereas the elimination of beta emitters was about 35%. Overall, the data provided evidence that the pilot plant is effective for removing different radionuclides that can be present in the incoming water treated. Therefore, tertiary treatment based on reverse osmosis has a positive effect in water quality.

Systematic study of probable projectile-target combinations for the synthesis of the superheavy nucleus 302120

NASA Astrophysics Data System (ADS)

Santhosh, K. P.; Safoora, V.

2016-08-01

Probable projectile-target combinations for the synthesis of the superheavy element 302120 have been studied taking the Coulomb and proximity potential as the interaction barrier. The probabilities of the compound nucleus formation PCN for the projectile-target combinations found in the cold reaction valley of 302120 are estimated. At energies near and above the Coulomb barrier, we have calculated the capture, fusion, and evaporation residue cross sections for the reactions of all probable projectile-target combinations so as to predict the most promising projectile-target combinations for the synthesis of the superheavy element 302120 in heavy-ion fusion reactions. The calculated fusion and evaporation cross sections for the more asymmetric ("hotter") projectile-target combination is found to be higher than the less asymmetric ("colder") combination. It can be seen from the nature of the quasifission barrier height, mass asymmetry, the probability of compound nucleus formation, survival probability, and excitation energy, the systems 44Ar+258No , 46Ar+256No , 48Ca+254Fm , 50Ca+252Fm , 54Ti+248Cf , and 58Cr+244Cm in deep region I of the cold reaction valley and the systems 62Fe+240Pu , 64Fe+238Pu , 68Ni+234U , 70Ni+232U , 72Ni+230U , and 74Zn+228Th in the other cold valleys are identified as the better projectile-target combinations for the synthesis of 302120. Our predictions on the synthesis of 302120 superheavy nuclei using the combinations 54Cr+248Cm , 58Fe+244Pu , 64Ni+238U , and 50Ti+249Cf are compared with available experimental data and other theoretical predictions.

The efficacy of denaturing actinide elements as a means of decreasing materials attractiveness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hase, K.R.; Bathke, C.G.; Ebbinghaus, B.B.

2013-07-01

This study considers the concept of denaturing as applied to the actinide elements present in spent fuel as a means to reduce materials attractiveness. Highly attractive materials generally have low values of bare critical mass, heat content, and dose. To denature an attractive element, its spent-fuel isotopic composition (isotopic vector) is intentionally modified by introducing sufficient quantities of a significantly less attractive isotope to dilute the concentration of a highly attractive isotope so that the overall attractiveness of the element is reduced. The authors used FOM (Figure of Merit) formula as the material attractiveness metric for their parametric determination ofmore » the attractiveness of the Pu and U. Materials attractiveness needs to be considered in three distinct phases in the process to construct a nuclear explosive device (NED): the acquisition phase, processing phase, and utilization phase. The results show that denaturing uranium with {sup 238}U is actually an effective means of reducing the attractiveness. For uranium with a large minority of {sup 235}U, a mixture of 80% {sup 238}U to 20% {sup 235}U is required to reduce the attractiveness to low. For uranium with a large concentration of {sup 233}U, a mixture of 88% {sup 238}U to 12% {sup 233}U is required to reduce the attractiveness to low. The results also show that denaturing plutonium with {sup 238}Pu is less effective than denaturing uranium with {sup 238}U. Using {sup 238}Pu as the denaturing agent would require 80% or more by mass in order to reduce the attractiveness to low. No amount of {sup 240}Pu is enough to reduce the plutonium attractiveness below medium. The combination of {sup 238}Pu and {sup 240}Pu would require approximately 70% {sup 238}Pu and 25% {sup 240}Pu by mass to reduce the plutonium attractiveness to low.« less

Compendium of energy-dependent sensitivity profiles for the TRX-2 thermal lattice

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tomlinson, E.T.; Lucius, J.L.; Drischler, J.D.

1978-03-01

Energy-dependent sensitivity profiles for five responses calculated for the TRX-2 thermal lattice with the ORNL sensitivity code system FORSS are presented here both in graphical form and in SENPRO format. The responses are the multiplication factor, k/sub eff/; the ratio of epithermal-to-thermal captures in /sup 238/U, /sup 28/rho; the ratio of epithermal-to-thermal fissions in /sup 235/U, /sup 25/delta; the ratio of fissions in /sup 238/U to fissions in /sup 235/U, /sup 28/delta; and the ratio of captures in /sup 238/U to fissions in /sup 235/U, CR. A summary table of the total sensitivities is also presented.

Recent results in nucleocosmochronology

NASA Astrophysics Data System (ADS)

Cowan, John J.; Thielemann, F.-K.; Truran, J. W.

Rates for beta-delayed neutron emission and fission have recently been calculated for the mass range 70-100. Using these new rates and the calculated rates for neutron capture, photodisintegration and beta decay, dynamical r-process calculations have been performed. For certain assumed conditions, these r-process calculations give a good fit to the solar system r-process abundance curve. These calculations have been used to obtain new production ratios for the nuclear chronometer pairs used to determine the age of the Galaxy - (Th-232)/(U-238) = 1.60, (U-235)/(U-238) = 1.16, and (Pu-244)/(U-238) = 0.40. Using the new production ratio for (Th-232)/(U-238) and (U-235)/(U238), with the observed meteoritic values for these nuclei and assuming a model of chemical evolution of the Galaxy, the age of the Galaxy has been determined. The results depend upon the initial nucleosynthesis enrichment in the Galactic disk, S0. While there are uncertainties in the calculations for a range of S0 from 0.1 to 0.3 (i.e., from 10 to 30 percent), the age of the Galaxy is found to be 12.4-14.7 Gyr.

Measurements of natural uranium concentration and isotopic composition with permil-level precision by inductively coupled plasma-quadrupole mass spectrometry

NASA Astrophysics Data System (ADS)

Shen, Chuan-Chou; Lin, Huei-Ting; Chu, Mei-Fei; Yu, Ein-Fen; Wang, Xianfeng; Dorale, Jeffrey A.

2006-09-01

A new analytical technique using inductively coupled plasma-quadrupole mass spectrometry (ICP-QMS) has been developed that produces permil-level precision in the measurement of uranium concentration ([U]) and isotopic composition (δ234U) in natural materials. A 233U-236U double spike method was used to correct for mass fractionation during analysis. To correct for ratio drifting, samples were bracketed by uranium standard measurements. A sensitivity of 6-7 × 108 cps/ppm was generated with a sample solution uptake rate of 30 μL/min. With a measurement time of 15-20 min, standards of 30-ng uranium produced a within-run precision better than 3‰ (±2 R.S.D.) for δ234U and better than 2‰ for [U]. Replicate measurements made on standards show that a between-run reproducibility of 3.5‰ for δ234U and 2‰ for [U] can be achieved. ICP-QMS data of δ234U and [U] in seawater, coral, and speleothem materials are consistent with the data measured by other ICP-MS and TIMS techniques. Advantages of the ICP-QMS method include low cost, easy maintenance, simple instrumental operation, and few sample preparation steps. Sample size requirements are small, such as 10-14 mg of coral material. The results demonstrate that this technique can be applied to natural samples with various matrices.

Empirical calibration of uranium releases in the terrestrial environment of nuclear fuel cycle facilities.

PubMed

Pourcelot, Laurent; Masson, Olivier; Saey, Lionel; Conil, Sébastien; Boulet, Béatrice; Cariou, Nicolas

2017-05-01

In the present paper the activity of uranium isotopes measured in plants and aerosols taken downwind of the releases of three nuclear fuel settlements was compared between them and with the activity measured at remote sites. An enhancement of 238 U activity as well as 235 U/ 238 U anomalies and 236 U are noticeable in wheat, grass, tree leaves and aerosols taken at the edge of nuclear fuel settlements, which show the influence of uranium chronic releases. Further plants taken at the edge of the studied sites and a few published data acquired in the same experimental conditions show that the 238 U activity in plants is influenced by the intensity of the U atmospheric releases. Assuming that 238 U in plant is proportional to the intensity of the releases, we proposed empirical relationships which allow to characterize the chronic releases on the ground. Other sources of U contamination in plants such as accidental releases and "delayed source" of uranium in soil are also discussed in the light of uranium isotopes signatures. Copyright © 2017 Elsevier Ltd. All rights reserved.

Quantification of 235U and 238U activity concentrations for undeclared nuclear materials by a digital gamma-gamma coincidence spectroscopy.

PubMed

Zhang, Weihua; Yi, Jing; Mekarski, Pawel; Ungar, Kurt; Hauck, Barry; Kramer, Gary H

2011-06-01

The purpose of this study is to investigate the possibility of verifying depleted uranium (DU), natural uranium (NU), low enriched uranium (LEU) and high enriched uranium (HEU) by a developed digital gamma-gamma coincidence spectroscopy. The spectroscopy consists of two NaI(Tl) scintillators and XIA LLC Digital Gamma Finder (DGF)/Pixie-4 software and card package. The results demonstrate that the spectroscopy provides an effective method of (235)U and (238)U quantification based on the count rate of their gamma-gamma coincidence counting signatures. The main advantages of this approach over the conventional gamma spectrometry include the facts of low background continuum near coincident signatures of (235)U and (238)U, less interference from other radionuclides by the gamma-gamma coincidence counting, and region-of-interest (ROI) imagine analysis for uranium enrichment determination. Compared to conventional gamma spectrometry, the method offers additional advantage of requiring minimal calibrations for (235)U and (238)U quantification at different sample geometries. Crown Copyright © 2011. Published by Elsevier Ltd. All rights reserved.

U-series vs 14C ages of deep-sea corals from the southern Labrador Sea: Sporadic development of corals and geochemical processes hampering estimation of ambient water ventilation ages

NASA Astrophysics Data System (ADS)

Hillaire-Marcel, Claude; Maccali, Jenny; Ménabréaz, Lucie; Ghaleb, Bassam; Blénet, Aurélien; Edinger, Evan

2017-04-01

Deep-sea scleractinian corals were collected with the remotely operated ROPOS vehicle off Newfounland. Fossil specimens of Desmophyllum dianthus were raised from coral graveyards at Orphan Knoll (˜1700m depth) and Flemish cap (˜2200 m depth), while live specimens were collected directly in overlying steep rock slopes. D. dianthus has an aragonitic skeleton and is thus particularly suited for U-Th dating. We obtained > 70 U-series ages along with > 20 14C measurements. Results display a discrete age distribution with two age clusters: a Bølling-Allerød and Holocene cluster with > 20 samples, and a Marine Isotope Stage (MIS) 5c cluster with ˜50 samples. Only two samples lay outside these clusters, at ˜ 64 ka and at ˜181 ka. Contrary to the New England seamounts where coral presence seems to have been continue through the last 70 ka, Orphan Knoll and Flemish Cap graveyards are marked by the absence of preserved specimens from MIS 2 to MIS 4 and throughout MIS 6. For filter-feeding deep-sea corals, access to food-rich waters is essential. Hence the Holocene and MIS 5 clusters observed in the Labrador basin might represent intervals linked to high food availability, either through production in the overlying water column, more effectively in relation to particulate and dissolved organic carbon transport via an active Western Boundary Undercurrent. Comparison of 230Th-ages vs 14C-ages in order to document changes in ventilation ages of the ambient water masses is equivocal due to the presence of some diagenetic and/or initial 230Th-excess. In addition, discrete diagenetic U-fluxes can be documented from 234U/238U vs 230Th/238U data. They point to a recent winnowing of sediment overlying the fossil corals that we link to the Holocene intensification of the Western Boundary Undercurrent, which resulted in driving Fe-Mn coatings.

Uranium isotope ratios of Muonionalusta troilite and complications for the absolute age of the IVA iron meteorite core

NASA Astrophysics Data System (ADS)

Brennecka, Gregory A.; Amelin, Yuri; Kleine, Thorsten

2018-05-01

The crystallization ages of planetary crustal material (given by basaltic meteorites) and planetary cores (given by iron meteorites) provide fiducial marks for the progress of planetary formation, and thus, the absolute ages of these objects fundamentally direct our knowledge and understanding of planet formation and evolution. The lone precise absolute age of planetary core material was previously obtained on troilite inclusions from the IVA iron meteorite Muonionalusta. This previously reported Pb-Pb age of 4565.3 ± 0.1 Ma-assuming a 238U/235U =137.88-only post-dated the start of the Solar System by approximately 2-3 million years, and mandated fast cooling of planetary core material. Since an accurate Pb-Pb age requires a known 238U/235U of the sample, we have measured both 238U/235U and Pb isotopic compositions of troilite inclusions from Muonionalusta. The measured 238U/235U of the samples range from ∼137.84 to as low as ∼137.22, however based on Pb and U systematics, terrestrial contamination appears pervasive and has affected samples to various extents for Pb and U. The cause of the relative 235U excess in one sample does not appear to be from terrestrial contamination or the decay of short-lived 247Cm, but is more likely from fractionation of U isotopes during metal-silicate separation during core formation, exacerbated by the extreme U depletion in the planetary core. Due to limited Pb isotopic variation and terrestrial disturbance, no samples of this study produced useful age information; however the clear divergence from the previously assumed 238U/235U of any troilite in Muonionalusta introduces substantial uncertainty to the previously reported absolute age of the sample without knowledge of the 238U/235U of the sample. Uncertainties associated with U isotope heterogeneity do not allow for definition of a robust age of solidification and cooling for the IVA core. However, one sample of this work-paired with previous work using short-lived radionuclides-suggests that the cooling age of the IVA core may be significantly younger than previously thought. This work indicates the metallic cores of protoplanetary bodies solidified no earlier than the first ∼5-10 million years of the Solar System.

Evaluation of annual committed effective doses to members of the public in Morocco due to 238U and 232Th in various food materials.

PubMed

Misdaq, M A; Bourzik, W

2004-12-01

Uranium (238U) and thorium (232Th) concentrations were measured in different foods widely consumed in Morocco by using CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs). Annual committed effective doses due to 238U and 232Th intakes from the ingestion of the studied food materials were evaluated for different age groups of individuals, using the ICRP ingestion dose coefficients. The influence of the 238U and 232Th intakes and ages of individuals on the committed effective dose was investigated. Total annual intakes of 238U and 232Th for a typical food basket for adult members of the Moroccan population were estimated to be 451 +/- 27 Bq y(-1) and 359 +/- 20 Bq y(-1), corresponding to committed effective doses of (20 +/- 1) x 10(-6) Sv y(-1) and (83 +/- 5) x 10(-6) Sv y(-1), respectively.

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.

National low-level waste management program radionuclide report series, Volume 15: Uranium-238

DOE Office of Scientific and Technical Information (OSTI.GOV)

Adams, J.P.

1995-09-01

This report, Volume 15 of the National Low-Level Waste Management Program Radionuclide Report Series, discusses the radiological and chemical characteristics of uranium-238 ({sup 238}U). The purpose of the National Low-Level Waste Management Program Radionuclide Report Series is to provide information to state representatives and developers of low-level radioactive waste disposal facilities about the radiological, chemical, and physical characteristics of selected radionuclides and their behavior in the waste disposal facility environment. This report also includes discussions about waste types and forms in which {sup 238}U can be found, and {sup 238}U behavior in the environment and in the human body.

Annual committed effective dose from olive oil (due to 238U, 232Th, and 222Rn) estimated for members of the Moroccan public from ingestion and skin application.

PubMed

Misdaq, M A; Touti, R

2012-03-01

Olive oil is traditionally refined and widely consumed by Moroccan rural populations. Uranium (238U), thorium (232Th), radon (222Rn), and thoron (220Rn) contents were measured in various locally produced olive oil samples collected in rural areas of Morocco. These radionuclides were also measured inside various bottled virgin olive oils consumed by the Moroccan populations. CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs) were used. Annual committed effective doses due to 238U, 232Th, and 222Rn from the ingestion of olive oil by the members of the general public were determined. The maximum total committed effective dose due to 238U, 232Th, and 222Rn from the ingestion of olive oil by adult members of Moroccan rural populations was found equal to 5.9 µSv y-1. The influence of pollution due to building material dusts and phosphates on the radiation dose to workers from the ingestion of olive oil was investigated, and it was found that the maximum total committed effective dose due to 238U, 232Th, and 222Rn was on the order of 0.22 mSy y-1. Committed effective doses to skin due to 238U, 232Th, and 222Rn from the application of olive oil masks by rural women were evaluated. The maximum total committed effective dose to skin due to 238U, 232Th, and 222Rn was found equal to 0.07 mSy y-1 cm-2.

Determination of uranium isotopic composition and 236U content of soil samples and hot particles using inductively coupled plasma mass spectrometry.

PubMed

Boulyga, S F; Becker, J S

2001-07-01

As a result of the accident at the Chernobyl nuclear power plant (NPP) the environment was contaminated with spent nuclear fuel. The 236U isotope was used in this study to monitor the spent uranium from nuclear fallout in soil samples collected in the vicinity of the Chernobyl NPP. Nuclear track radiography was applied for the identification and extraction of hot radioactive particles from soil samples. A rapid and sensitive analytical procedure was developed for uranium isotopic ratio measurement in environmental samples based on double-focusing inductively coupled plasma mass spectrometry (DF-ICP-MS) with a MicroMist nebulizer and a direct injection high-efficiency nebulizer (DIHEN). The performance of the DF-ICP-MS with a quartz DIHEN and plasma shielded torch was studied. Overall detection efficiencies of 4 x 10(-4) and 10(-3) counts per atom were achieved for 238U in DF-ICP-QMS with the MicroMist nebulizer and DIHEN, respectively. The rate of formation of uranium hydride ions UH+/U+ was 1.2 x 10(-4) and 1.4 x 10(-4), respectively. The precision of short-term measurements of uranium isotopic ratios (n = 5) in 1 microg L(-1) NBS U-020 standard solution was 0.11% (238U/235U) and 1.4% (236U/238U) using a MicroMist nebulizer and 0.25% (235U/238U) and 1.9% (236U/P38U) using a DIHEN. The isotopic composition of all investigated Chernobyl soil samples differed from those of natural uranium; i.e. in these samples the 236U/238U ratio ranged from 10(-5) to 10(-3). Results obtained with ICP-MS, alpha- and gamma-spectrometry showed differences in the migration properties of spent uranium, plutonium, and americium. The isotopic ratio of uranium was also measured in hot particles extracted from soil samples.

Measurement of the normalized 238U(n ,f )/235U(n ,f ) cross section ratio from threshold to 30 MeV with the NIFFTE fission Time Projection Chamber

NASA Astrophysics Data System (ADS)

Casperson, R. J.; Asner, D. M.; Baker, J.; Baker, R. G.; Barrett, J. S.; Bowden, N. S.; Brune, C.; Bundgaard, J.; Burgett, E.; Cebra, D. A.; Classen, T.; Cunningham, M.; Deaven, J.; Duke, D. L.; Ferguson, I.; Gearhart, J.; Geppert-Kleinrath, V.; Greife, U.; Grimes, S.; Guardincerri, E.; Hager, U.; Hagmann, C.; Heffner, M.; Hensle, D.; Hertel, N.; Higgins, D.; Hill, T.; Isenhower, L. D.; King, J.; Klay, J. L.; Kornilov, N.; Kudo, R.; Laptev, A. B.; Loveland, W.; Lynch, M.; Lynn, W. S.; Magee, J. A.; Manning, B.; Massey, T. N.; McGrath, C.; Meharchand, R.; Mendenhall, M. P.; Montoya, L.; Pickle, N. T.; Qu, H.; Ruz, J.; Sangiorgio, S.; Schmitt, K. T.; Seilhan, B.; Sharma, S.; Snyder, L.; Stave, S.; Tate, A. C.; Tatishvili, G.; Thornton, R. T.; Tovesson, F.; Towell, D. E.; Towell, R. S.; Walsh, N.; Watson, S.; Wendt, B.; Wood, L.; Yao, L.; Younes, W.; Niffte Collaboration

2018-03-01

The normalized 238U(n ,f )/235U(n ,f ) cross section ratio has been measured using the NIFFTE fission Time Projection Chamber (fissionTPC) from the reaction threshold to 30 MeV . The fissionTPC is a two-volume MICROMEGAS time projection chamber that allows for full three-dimensional reconstruction of fission-fragment ionization profiles from neutron-induced fission. The measurement was performed at the Los Alamos Neutron Science Center, where the neutron energy is determined from neutron time of-flight. The 238U(n ,f )/235U(n ,f ) ratio reported here is the first cross section measurement made with the fissionTPC, and will provide new experimental data for evaluation of the 238U(n ,f ) cross section, an important standard used in neutron-flux measurements. Use of a development target in this work prevented the determination of an absolute normalization, to be addressed in future measurements. Instead, the measured cross section ratio has been normalized to ENDF/B-VIII.β 5 at 14.5 MeV.

Determination of 235U/238U Ratio on Urine by ICP-MS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Collins, L; Gobaleza, A; Langston, R

2011-10-19

LLNL Internal Dosimetry Program - The new procedure satisfies the requirement to determine {sup 235}U/{sup 238}U ratio in bioassay urine samples. MDA - The L{sub C} and MDA{sub 95} for {sup 235}U are well below the required detection limit of 0.00035 {mu}g/L. Turn around time - Analysis of 10 samples plus 2 QCs can be completed in one work day (8 hours).

Estimation of annual effective dose due to ingestion of natural radionuclides in foodstuffs and water at a proposed uranium mining site in India.

PubMed

Giri, Soma; Jha, V N; Singh, Gurdeep; Tripathi, R M

2013-12-01

To study the distribution of (210)Po, (226)Ra, (230)Th and U(nat) (naturally occurring radioisotopes of uranium [(234)U, (235)U and (238)U]) in food and water around the Bagjata uranium mining area in India. Radionuclides were analyzed in food samples of plant and animal origin after acid digestion. Intake and ingestion dose of the radionuclides were estimated. (210)Po, (226)Ra, (230)Th and U(nat) in all the dietary components ranged widely from < 0.2-36, < 0.02-1.58, < 0.01-2.8 and < 0.017-0.39 Bqkg(-1), respectively. The range of (226)Ra and U(nat) in water was < 3.5-206 and < 12.6-693 mBql(-1), respectively. The intake of radionuclides considering food and water was calculated to be 760 BqY(-1) while the ingestion dose was 601 μSvY(-1). The estimated doses reflect the natural background dose via route of ingestion, which is below the 1 mSvY(-1) limit set by the International Commission on Radiological Protection (ICRP). However, the doses are more than the dose constraint of 300 μSvY(-1) as suggested by the ICRP for members of the public for planned disposal of long-lived radioactive waste. The study confirms that current levels of radionuclides do not pose significant radiological risk to the local inhabitants, but they need close investigation in the near future.

Sea-level history and tectonic uplift during the last-interglacial period (LIG): Inferred from the Bab al-Mandab coral reef terraces, southern Red Sea

NASA Astrophysics Data System (ADS)

Al-Mikhlafi, Ahmed Saif; Edwards, Lawrence R.; Cheng, Hai

2018-02-01

Results of U-series dating of late Pleistocene raised coral reef terraces from the Bab al-Mandab area, define two distinct groups: (1) well-preserved aragonitic fossil corals recorded from the Al-Hajaja terrace (Tr3) yield ages for last-interglacial period (LIG); and (2) calcitic fossil corals recovered from Perim Island terrace (Tr1) show varying degrees of U-series open system behavior and yield coral assemblage ages of LIG and older ages. Fossil corals from Tr1 are recrystallized corals, have anomalously high initial δ234U ranged from (152 ± 2‰ to 287 ± 7‰), corresponding to ages of ∼120 ka and ∼406 ka, respectively. Applying age reliability criteria on the current data suggest majority of the ages cannot be considered reliable and all are suspected for open system behavior associated with U loss/addition that significantly affects the 230Th/U ages. The diagenesis shown by these corals occurred probably due to extensive interaction of fossil corals with freshwater during the wet periods prevailed in southern Arabia coeval with the African monsoon, which led to U loss. Post-depositional U loss suggest (230Th/238U) increase, which shift the U-Th ages to unexpectedly higher levels as it is shown here. Measured elevation at the Al-Hajaja terrace (Tr3) is ∼4 ± 2 m above present sea level (apsl) consistent with eustatic sea level changes and indicates that the Bab al-Mandab area is stable at least since the LIG period. The Perim Island terrace (Tr1) is at elevation of 7 ± 2 m apsl; its reef yields diageneticaly-altered corals of multiple ages and cannot be used for sea level reconstructions.

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 abiotic CaCO3 reflect changes in aqueous U(VI) speciation, which are in turn a function of carbonate ion chemistry and pH. Hence, the door is opened to the development of a possible 238U/235U proxy for the carbonate ion system. [1] DeCarlo et al., (2015), GCA, 162,151-165. [2] Reeder et a., (2001), GCA, 65, 3491-3503. [3] Weyer et al., (2008) GCA 72, 345-359.

Radioactive Contamination of Alluvial Soils in the Taiga Landscapes of Yakutia with 137Cs, 226Ra, and 238U

NASA Astrophysics Data System (ADS)

Chevychelov, A. P.; Sobakin, P. I.

2017-12-01

The concentrations and distribution of 137Cs in alluvial soils (Fluvisols) of the upper and middle reaches of the Markha River in the northwest of Yakutia and 226Ra and 238U in alluvial soils within the El'kon uranium ore deposit in the south of Yakutia have been studied. It is shown that the migration of radiocesium in the permafrost-affected soils of Yakutia owing to alluviation processes extends to more than 600 km from the source of the radioactive contamination. The migration of 137Cs with water flows is accompanied by its deposition in the buried horizons of alluvial soils during extremely high floods caused by ice jams. In the technogenic landscapes of southern Yakutia, active water migration of 238U and 226Ra from radioactive dump rocks. The leaching of 238U with surface waters from the rocks is more intense than the leaching of 226Ra. The vertical distribution patterns of 238U and 226Ra in the profiles of alluvial soils are complex. Uranium tends to accumulate in the surface humus horizon and in the buried soil horizons, whereas radium does not display any definite regularities of its distribution in the soil profiles. At present, the migration of 238U and 226Ra with river water and their accumulation in the alluvial soils extend to about 30 km from the source.

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.

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 product U(VI) ~0.1‰ heavier than the remaining UO2. We attribute the lack of strong fractionation during oxidation of solid UO2 to a 'rind effect', where the surface layer must be completely oxidized before the next layer is exposed to oxidant. Hence, nearly complete, congruent conversion of each layer of U(IV) to U(VI) results in minimal isotope fractionation. A small amount of transient fractionation probably occurs initially, but this is quickly negated as the surface becomes isotopically fractionated. Interestingly, our measured ~0.1‰ U isotope fractionation during oxidation of solid U(IV) agrees with the natural observation that 238U/235U ratios in river water (mainly U(VI)) are ~0.1‰ greater than those in fresh continental rocks (primarily U(IV) minerals). Application of these results to natural settings should be done with caution, however. Oxidation of natural uraninite in continental rocks is a much slower process. If the U(VI) product and the U(IV) reactant remain in contact for long periods of time (e.g., months), they may evolve toward isotopic equilibrium. Measurements of 238U/235U in various natural weathering environments should be undertaken to examine this idea.

(234)Th as a tracer of vertical transport of polycyclic aromatic hydrocarbons in the northern Gulf of Mexico.

PubMed

Adhikari, Puspa L; Maiti, Kanchan; Bosu, Somiddho; Jones, Patrick R

2016-06-15

Particle-mediated vertical flux of polycyclic aromatic hydrocarbons (PAHs) plays an important role in their removal from upper oceans and sets a limit on the amount delivered to the deep-sea sediments. In this study, we applied a one-dimensional steady-state (234)Th scavenging model to estimate vertical flux of PAHs in the northern Gulf of Mexico and compared them with sediment trap based flux estimates. The (234)Th-based ∑PAH43 fluxes were 6.7±1.0μgm(-2)d(-1) and 3.7±0.6μgm(-2)d(-1) while sediment trap-based fluxes were 4.0±0.6μgm(-2)d(-1) and 4.5±0.7μgm(-2)d(-1) at 150m and 250m, respectively. Alkylated homologues contributed to 80% of the total PAH fluxes which is in contrary to other regions where combustion derived parent PAHs dominate the fluxes. The results indicate that the (238)U-(234)Th disequilibria can be an effective tracer of particulate PAH fluxes in upper mesopelagic zones and can provide flux estimates with high spatial coverage needed to quantify their long term fate and transport in the marine systems. Copyright © 2016 Elsevier Ltd. All rights reserved.

Enhanced nucleon transfer in tip collisions of 238U+124Sn

NASA Astrophysics Data System (ADS)

Sekizawa, Kazuyuki

2017-10-01

Multinucleon transfer processes in low-energy heavy ion reactions have attracted increasing interest in recent years aiming at the production of new neutron-rich isotopes. Clearly, it is an imperative task to further develop understanding of underlying reaction mechanisms to lead experiments to success. In this paper, from systematic time-dependent Hartree-Fock calculations for the 238U+124Sn reaction, it is demonstrated that transfer dynamics depend strongly on the orientations of 238U, quantum shells, and collision energies. Two important conclusions are obtained: (i) Experimentally observed many-proton transfer from 238U to 124Sn can be explained by a multinucleon transfer mechanism governed by enhanced neck evolution in tip collisions; (ii) novel reaction dynamics are observed in tip collisions at energies substantially above the Coulomb barrier, where a number of nucleons are transferred from 124Sn to 238U, producing transuranium nuclei as primary reaction products, which could be a means to synthesize superheavy nuclei. Both results indicate the importance of the neck (shape) evolution dynamics, which are sensitive to orientations, shell effects, and collision energies, for exploring possible pathways to produce new unstable nuclei.

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 microsamples varied in the range from 0.0073 (corresponding to the natural uranium isotopic composition) to 0.023 (corresponding to initial 235U enrichment in reactor fuel). An inverse correlation was observed between the 236U/238U and 235U/238U isotope ratios, except in the case of one sample with natural uranium. The heterogeneity of the uranium isotope composition is attributed to the different burn-up grades of uranium in the fuel rods from which the microsamples originated.

Nuclear reactor for breeding U.sup.233

DOEpatents

Bohanan, Charles S.; Jones, David H.; Raab, Jr., Harry F.; Radkowsky, Alvin

1976-01-01

A light-water-cooled nuclear reactor capable of breeding U.sup.233 for use in a light-water breeder reactor includes physically separated regions containing U.sup.235 fissile material and U.sup.238 fertile material and Th.sup.232 fertile material and Pu.sup.239 fissile material, if available. Preferably the U.sup.235 fissile material and U.sup.238 fertile material are contained in longitudinally movable seed regions and the Pu.sup.239 fissile material and Th.sup.232 fertile material are contained in blanket regions surrounding the seed regions.

Analysis of the natural radioactivity concentrations of the fine dust samples in Jeju Island, Korea and the annual effective radiation dose by inhalation.

PubMed

Han, Chung Hun; Park, Jae Woo

2018-01-01

This study analyzed the concentrations of potassium, thorium and uranium of the atmospheric PM 10 aerosols which were collected at Gosan of Jeju Island during the year of 2014. The mean mass concentration of PM 10 was 47.31 μg/m 3 . The mean radioactive concentrations of 40 K, 232 Th and 238 U were 7.89, 0.25 and 0.30 μBq/m 3 , respectively. The 232 Th/ 238 U activity concentration ratio of PM 10 was 0.830. The 232 Th/ 238 U ratio during Asian Dust days is 1.073, which is higher than those in other atmospheric conditions. The concentration ratio of 232 Th/ 238 U was 0.902 in China continent.

IAEA CIELO Evaluation of Neutron-induced Reactions on 235U and 238U Targets

DOE PAGES

Capote, R.; Trkov, A.; Sin, M.; ...

2018-02-01

Evaluations of nuclear reaction data for the major uranium isotopes 238U and 235U were performed within the scope of the CIELO Project on the initiative of the OECD/NEA Data Bank under Working Party on Evaluation Co-operation (WPEC) Subgroup 40 coordinated by the IAEA Nuclear Data Section. Both the mean values and covariances are evaluated from 10 -5 eV up to 30 MeV. The resonance parameters of 238U and 235U were re-evaluated with the addition of newly available data to the existing experimental database. The evaluations in the fast neutron range are based on nuclear model calculations with the code EMPIRE–3.2more » Malta above the resonance range up to 30 MeV. 235U(n,f), 238U(n,f), and 238U(n,γ) cross sections and 235U(n th,f) prompt fission neutron spectrum (PFNS) were evaluated within the Neutron Standards project and are representative of the experimental state-of-the-art measurements. The Standards cross sections were matched in model calculations as closely as possible to guarantee a good predictive power for cross sections of competing neutron scattering channels. 235U(n,γ) cross section includes fluctuations observed in recent experiments. 235U(n,f) PFNS for incident neutron energies from 500 keV to 20 MeV were measured at Los Alamos Chi-Nu facility and re-evaluated using all available experimental data. While respecting the measured differential data, several compensating errors in previous evaluations were identified and removed so that the performance in integral benchmarks was restored or improved. Covariance matrices for 235U and 238U cross sections, angular distributions, spectra and neutron multiplicities were evaluated using the GANDR system that combines experimental data with model uncertainties. Unrecognized systematic uncertainties were considered in the uncertainty quantification for fission and capture cross sections above the thermal range, and for neutron multiplicities. Evaluated files were extensively benchmarked to ensure good performance in reactor calculations and fusion-related systems. New comprehensive evaluations show excellent agreement with available differential data and integral performance better than current evaluated data libraries, and represent a step forward in a quest for better nuclear data for applications.« less

IAEA CIELO Evaluation of Neutron-induced Reactions on 235U and 238U Targets

NASA Astrophysics Data System (ADS)

Capote, R.; Trkov, A.; Sin, M.; Pigni, M. T.; Pronyaev, V. G.; Balibrea, J.; Bernard, D.; Cano-Ott, D.; Danon, Y.; Daskalakis, A.; Goričanec, T.; Herman, M. W.; Kiedrowski, B.; Kopecky, S.; Mendoza, E.; Neudecker, D.; Leal, L.; Noguere, G.; Schillebeeckx, P.; Sirakov, I.; Soukhovitskii, E. S.; Stetcu, I.; Talou, P.

2018-02-01

Evaluations of nuclear reaction data for the major uranium isotopes 238U and 235U were performed within the scope of the CIELO Project on the initiative of the OECD/NEA Data Bank under Working Party on Evaluation Co-operation (WPEC) Subgroup 40 coordinated by the IAEA Nuclear Data Section. Both the mean values and covariances are evaluated from 10-5 eV up to 30 MeV. The resonance parameters of 238U and 235U were re-evaluated with the addition of newly available data to the existing experimental database. The evaluations in the fast neutron range are based on nuclear model calculations with the code EMPIRE-3.2 Malta above the resonance range up to 30 MeV. 235U(n,f), 238U(n,f), and 238U(n,γ) cross sections and 235U(nth,f) prompt fission neutron spectrum (PFNS) were evaluated within the Neutron Standards project and are representative of the experimental state-of-the-art measurements. The Standards cross sections were matched in model calculations as closely as possible to guarantee a good predictive power for cross sections of competing neutron scattering channels. 235U(n,γ) cross section includes fluctuations observed in recent experiments. 235U(n,f) PFNS for incident neutron energies from 500 keV to 20 MeV were measured at Los Alamos Chi-Nu facility and re-evaluated using all available experimental data. While respecting the measured differential data, several compensating errors in previous evaluations were identified and removed so that the performance in integral benchmarks was restored or improved. Covariance matrices for 235U and 238U cross sections, angular distributions, spectra and neutron multiplicities were evaluated using the GANDR system that combines experimental data with model uncertainties. Unrecognized systematic uncertainties were considered in the uncertainty quantification for fission and capture cross sections above the thermal range, and for neutron multiplicities. Evaluated files were extensively benchmarked to ensure good performance in reactor calculations and fusion-related systems. New comprehensive evaluations show excellent agreement with available differential data and integral performance better than current evaluated data libraries, and represent a step forward in a quest for better nuclear data for applications.

IAEA CIELO Evaluation of Neutron-induced Reactions on 235U and 238U Targets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Capote, R.; Trkov, A.; Sin, M.

Evaluations of nuclear reaction data for the major uranium isotopes 238U and 235U were performed within the scope of the CIELO Project on the initiative of the OECD/NEA Data Bank under Working Party on Evaluation Co-operation (WPEC) Subgroup 40 coordinated by the IAEA Nuclear Data Section. Both the mean values and covariances are evaluated from 10 -5 eV up to 30 MeV. The resonance parameters of 238U and 235U were re-evaluated with the addition of newly available data to the existing experimental database. The evaluations in the fast neutron range are based on nuclear model calculations with the code EMPIRE–3.2more » Malta above the resonance range up to 30 MeV. 235U(n,f), 238U(n,f), and 238U(n,γ) cross sections and 235U(n th,f) prompt fission neutron spectrum (PFNS) were evaluated within the Neutron Standards project and are representative of the experimental state-of-the-art measurements. The Standards cross sections were matched in model calculations as closely as possible to guarantee a good predictive power for cross sections of competing neutron scattering channels. 235U(n,γ) cross section includes fluctuations observed in recent experiments. 235U(n,f) PFNS for incident neutron energies from 500 keV to 20 MeV were measured at Los Alamos Chi-Nu facility and re-evaluated using all available experimental data. While respecting the measured differential data, several compensating errors in previous evaluations were identified and removed so that the performance in integral benchmarks was restored or improved. Covariance matrices for 235U and 238U cross sections, angular distributions, spectra and neutron multiplicities were evaluated using the GANDR system that combines experimental data with model uncertainties. Unrecognized systematic uncertainties were considered in the uncertainty quantification for fission and capture cross sections above the thermal range, and for neutron multiplicities. Evaluated files were extensively benchmarked to ensure good performance in reactor calculations and fusion-related systems. New comprehensive evaluations show excellent agreement with available differential data and integral performance better than current evaluated data libraries, and represent a step forward in a quest for better nuclear data for applications.« less

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. Copyright © 2016 Elsevier B.V. All rights reserved.

Direct Measurement of Initial 230TH/ 232TH Ratios in Central Texas Speleothems for More Accurate Age Determination

NASA Astrophysics Data System (ADS)

Wortham, B. E.; Banner, J. L.; James, E.; Loewy, S. L.

2013-12-01

Speleothems, calcite deposits in caves, preserve a record of climate in their growth rate, isotope ratios and trace element concentrations. These variables must be tied to precise ages to produce pre-instrumental records of climate. The 238U-234U- 230Th disequilibrium method of dating can yield precise ages if the amount of 230Th from the decay of radiogenic 238U can be constrained. 230Th in a speleothem calcite growth layer has two potential sources - 1) decay of radioactive 238U since the time of growth of the calcite layer; and 2) initial detrital 230Th, incorporated along with detrital 232Th, into the calcite layer at the time it grew. Although the calcite lattice does not typically incorporate Th, samples can contain impurities with relatively high Th contents. Initial 230Th/232Th is commonly estimated by assuming a source with bulk-Earth U/Th values in a state of secular equilibrium in the 238U-decay chain. The uncertainty in this 230Th/232Th estimate is also assumed, typically at +/-100%. Both assumptions contribute to uncertainty in ages determined for young speleothems. If the amount of initial detrital 230Th can be better quantified for samples or sites, then U-series ages will have smaller uncertainties and more precisely define the time series of climate proxies. This study determined the initial 230Th/232Th of modern calcite to provide more precise dates for central Texas speleothems. Calcite was grown on glass-plate substrates placed under active drips in central Texas caves. The 230Th/232Th of this modern calcite was determined using thermal ionization mass spectrometry. Results show that: 1) initial 230Th/232Th ratios can be accurately determined in these young samples and 2) measuring 230Th/232Th reduces the uncertainties in previously-determined ages on stalagmites from under the same drips. For example, measured initial 230Th/232Th in calcite collected on substrates from different locations in the cave at Westcave Preserve are 15.3 × 0.67 ppm, 14.6 × 0.83 ppm, 5.8 × 0.56 ppm, and 5.9 × 0.60 ppm, which are higher and more precise than the value commonly assumed for initial 230Th/232Th, 4.4 × 4.4 ppm. Soil sampled above Westcave, a potential source of detrital Th incorporated into speleothems, also has a high calculated 230Th/232Th. We calculate soil 230Th/232Th from measured U and Th concentrations of soil leachates (using DI water and ammonium acetate). Calculated 230Th/232Th for Westcave soils range from 0.39 to 28.4 ppm, which encompasses the range of initial 230Th/232Th values found in the modern calcite. Soil leachates from Natural Bridge Caverns and Inner Space Cavern were analyzed by the same method, yielding calculated 230Th/232Th ranging from 1.5 to 12.6 ppm (Natural Bridge), and from 1.43 to 272 ppm (Inner Space). Soil and calcite data indicate that the commonly assumed initial 230Th/232Th is not always applicable and that initial 230Th/232Th can be estimated more accurately by measuring Th isotope ratios in modern calcite and soils to determine speleothem U-series ages.

Round-robin 230Th– 234U age dating of bulk uranium for nuclear forensics

DOE PAGES

Gaffney, Amy M.; Hubert, Amélie; Kinman, William S.; ...

2015-07-30

We report that in an inter-laboratory measurement comparison study, four laboratories determined 230Th– 234U model ages of uranium certified reference material NBL U050 using isotope dilution mass spectrometry. The model dates determined by the participating laboratories range from 9 March 1956 to 19 October 1957, and are indistinguishable given the associated measurement uncertainties. These model ages are concordant with to slightly older than the known production age of NBL U050.

Round-robin 230Th– 234U age dating of bulk uranium for nuclear forensics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gaffney, Amy M.; Hubert, Amélie; Kinman, William S.

We report that in an inter-laboratory measurement comparison study, four laboratories determined 230Th– 234U model ages of uranium certified reference material NBL U050 using isotope dilution mass spectrometry. The model dates determined by the participating laboratories range from 9 March 1956 to 19 October 1957, and are indistinguishable given the associated measurement uncertainties. These model ages are concordant with to slightly older than the known production age of NBL U050.

238U, and its decay products, in grasses from an abandoned uranium mine

NASA Astrophysics Data System (ADS)

Childs, Edgar; Maskall, John; Millward, Geoffrey

2016-04-01

Bioaccumulation of radioactive contaminants by plants is of concern particularly where the sward is an essential part of the diet of ruminants. The abandoned South Terras uranium mine, south west England, had primary deposits of uraninite (UO2) and pitchblende (U3O8), which contained up to 30% uranium. When the mine was active uranium and radium were extracted but following closure it was abandoned without remediation. Waste rock and gangue, consisting of inefficiently processed minerals, were spread around the site, including a field where ruminants are grazed. Here we report the activity concentrations of 238U, 235U 214,210Pb, and the concentrations of selected metals in the soils, roots and leaves of grasses taken from the contaminated field. Soil samples were collected at the surface, and at 30 cm depth, using an auger along a 10-point transect in the field from the foot of a waste heap. Whole, individual grass plants were removed with a spade, ensuring that their roots were intact. The soils and roots and grass leaves were freeze-dried. Activity concentrations of the radionuclides were determined by gamma spectroscopy, following 30 days incubation for development of secular equilibrium. Dried soils, roots and grasses were also digested in aqua regia and the concentrations of elements determined by ICP techniques. Maximum activity concentrations of 238U, 235U, 214Pb and 210Pb surface soils were 63,300, 4,510, 23,300 and 49,400 Bq kg-1, respectively. The mean 238U:235U ratio was 11.8 ± 1.8, an order of magnitude lower than the natural value of 138, indicating disequilibrium within the decay chain due to mineral processing. Radionuclides in the roots had 5 times lower concentration and only grass leaves in the vicinity of the waste heap had measureable values. The mean soil to root transfer factor for 238U was 36%, the mean root to leaf was 3% and overall only 0.7% of 238U was transferred from the soil to the leaves. The roots contained 0.8% iron, possibly as iron plaque acting to mediate 238U transfer within the plants. The results are discussed in the context of remediation of grazing land contaminated with radionuclides.

Measurement of the normalized U 238 ( n , f ) / U 235 ( n , f ) cross section ratio from threshold to 30 MeV with the NIFFTE fission Time Projection Chamber

DOE PAGES

Casperson, R. J.; Asner, D. M.; Baker, J.; ...

2018-03-23

We present that the normalized 238U(n,f)/ 235U(n,f) cross section ratio has been measured using the NIFFTE fission Time Projection Chamber (fissionTPC) from the reaction threshold to 30 MeV . The fissionTPC is a two-volume MICROMEGAS time projection chamber that allows for full three-dimensional reconstruction of fission-fragment ionization profiles from neutron-induced fission. The measurement was performed at the Los Alamos Neutron Science Center, where the neutron energy is determined from neutron time of-flight. The 238U(n,f)/ 235U(n,f) ratio reported here is the first cross section measurement made with the fissionTPC, and will provide new experimental data for evaluation of the 238U(n,f) crossmore » section, an important standard used in neutron-flux measurements. Use of a development target in this work prevented the determination of an absolute normalization, to be addressed in future measurements. Instead, the measured cross section ratio has been normalized to ENDF/B-VIII.β5 at 14.5 MeV.« less

Measurement of the normalized U 238 ( n , f ) / U 235 ( n , f ) cross section ratio from threshold to 30 MeV with the NIFFTE fission Time Projection Chamber

DOE Office of Scientific and Technical Information (OSTI.GOV)

Casperson, R. J.; Asner, D. M.; Baker, J.

We present that the normalized 238U(n,f)/ 235U(n,f) cross section ratio has been measured using the NIFFTE fission Time Projection Chamber (fissionTPC) from the reaction threshold to 30 MeV . The fissionTPC is a two-volume MICROMEGAS time projection chamber that allows for full three-dimensional reconstruction of fission-fragment ionization profiles from neutron-induced fission. The measurement was performed at the Los Alamos Neutron Science Center, where the neutron energy is determined from neutron time of-flight. The 238U(n,f)/ 235U(n,f) ratio reported here is the first cross section measurement made with the fissionTPC, and will provide new experimental data for evaluation of the 238U(n,f) crossmore » section, an important standard used in neutron-flux measurements. Use of a development target in this work prevented the determination of an absolute normalization, to be addressed in future measurements. Instead, the measured cross section ratio has been normalized to ENDF/B-VIII.β5 at 14.5 MeV.« less

Uranium in agricultural soils and drinking water wells on the Swiss Plateau.

PubMed

Bigalke, Moritz; Schwab, Lorenz; Rehmus, Agnes; Tondo, Patrick; Flisch, Markus

2018-02-01

Mineral phosphorus fertilizers are regularly applied to agricultural sites, but their uranium (U) content is potentially hazardous to humans and the environment. Fertilizer-derived U can accumulate in the soil, but might also leach to ground-, spring and surface waters. We sampled 19 mineral fertilizers from the canton of Bern and soils of three arable and one forest reference sites at each of four locations with elevated U concentrations (7-28 μg L -1 ) in nearby drinking water wells. The total U concentrations of the fertilizers were measured. The soils were analysed at three depth intervals down to 1 m for general soil parameters, total Cd, P, U and NaHCO 3 -extractable U concentrations, and 234/238 U activity ratios (AR). The U concentrations and AR values of the drinking water samples were also measured. A theoretical assessment showed that fertilizer-derived U may cause high U concentrations in leaching waters (up to approx. 25 μg L -1 ), but normally contributes only a small amount (approx. 0-3 μg L -1 ). The arable soils investigated showed no significant U accumulation compared to the forest sites. The close positive correlation of AR with NaHCO 3 -extractable U (R = 0.7, p < 0.001) indicates that application of fertilizer can increase the extractable U pool. The lack of depth gradients in the soil U concentrations (1.5-2.7 mg kg -1 ) and AR (0.90-1.06) ratios are inconsistent with the accumulation of U in the surface soil, and might indicate some leaching of fertilizer-derived U. The AR values in the water samples were close to 1, possibly suggesting an influence of fertilizer-derived U. However, based on findings from the literature and considering the heterogeneity of the catchment area, the agricultural practices, and the comparatively long distance to the groundwater, we conclude that fertilizer-derived U makes only a minor contribution to the elevated U concentrations in the water samples. Copyright © 2017 Elsevier Ltd. All rights reserved.

Radionuclide inventories for the F- and H-area seepage basin groundwater plumes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hiergesell, Robert A; Kubilius, Walter P.

2016-05-01

Within the General Separations Areas (GSA) at the Savannah River Site (SRS), significant inventories of radionuclides exist within two major groundwater contamination plumes that are emanating from the F- and H-Area seepage basins. These radionuclides are moving slowly with groundwater migration, albeit more slowly due to interaction with the soil and aquifer matrix material. The purpose of this investigation is to quantify the activity of radionuclides associated with the pore water component of the groundwater plumes. The scope of this effort included evaluation of all groundwater sample analyses obtained from the wells that have been established by the Environmental Compliancemore » & Area Completion Projects (EC&ACP) Department at SRS to monitor groundwater contamination emanating from the F- and H-Area Seepage Basins. Using this data, generalized groundwater plume maps for the radionuclides that occur in elevated concentrations (Am-241, Cm-243/244, Cs-137, I-129, Ni-63, Ra-226/228, Sr-90, Tc-99, U-233/234, U-235 and U-238) were generated and utilized to calculate both the volume of contaminated groundwater and the representative concentration of each radionuclide associated with different plume concentration zones.« less

Use of ICP/MS with ultrasonic nebulizer for routine determination of uranium activity ratios in natural water

USGS Publications Warehouse

Kraemer, T.F.; Doughten, M.W.; Bullen, T.D.

2002-01-01

A method is described that allows precise determination of 234U/238U activity ratios (UAR) in most natural waters using commonly available inductively coupled plasma/mass spectrometry (ICP/MS) instrumentation and accessories. The precision achieved by this technique (??0.5% RSD, 1 sigma) is intermediate between thermal ionization mass spectrometry (??0.25% RSID, 1 sigma) and alpha particle spectrometry (??5% RSD, 1 sigma). It is precise and rapid enough to allow analysis of a large number of samples in a short period of time at low cost using standard, commercially available quadrupole instrumentation with ultrasonic nebulizer and desolvator accessories. UARs have been analyzed successfully in fresh to moderately saline waters with U concentrations of from less than 1 ??g/L to nearly 100 ??g/L. An example of the uses of these data is shown for a study of surface-water mixing in the North Platte River in western Nebraska. This rapid and easy technique should encourage the wider use of uranium isotopes in surface-water and groundwater investigations, both for qualitative (e.g. identifying sources of water) and quantitative (e.g. determining end-member mixing ratios purposes.

Geochemical and multi-isotopic (87Sr/86Sr, 143Nd/144Nd, 238U/235U) perspectives of sediment sources, depositional conditions, and diagenesis of the Marcellus Shale, Appalachian Basin, USA

NASA Astrophysics Data System (ADS)

Phan, Thai T.; Gardiner, James B.; Capo, Rosemary C.; Stewart, Brian W.

2018-02-01

We investigate sediment sources, depositional conditions and diagenetic processes affecting the Middle Devonian Marcellus Shale in the Appalachian Basin, eastern USA, a major target of natural gas exploration. Multiple proxies, including trace metal contents, rare earth elements (REE), the Sm-Nd and Rb-Sr isotope systems, and U isotopes were applied to whole rock digestions and sequentially extracted fractions of the Marcellus shale and adjacent units from two locations in the Appalachian Basin. The narrow range of εNd values (from -7.8 to -6.4 at 390 Ma) is consistent with derivation of the clastic sedimentary component of the Marcellus Shale from a well-mixed source of fluvial and eolian material of the Grenville orogenic belt, and indicate minimal post-depositional alteration of the Sm-Nd system. While silicate minerals host >80% of the REE in the shale, data from sequentially extracted fractions reflect post-depositional modifications at the mineralogical scale, which is not observed in whole rock REE patterns. Limestone units thought to have formed under open ocean (oxic) conditions have δ238U values and REE patterns consistent with modern seawater. The δ238U values in whole rock shale and authigenic phases are greater than those of modern seawater and the upper crust. The δ238U values of reduced phases (the oxidizable fraction consisting of organics and sulfide minerals) are ∼0.6‰ greater than that of modern seawater. Bulk shale and carbonate cement extracted from the shale have similar δ238U values, and are greater than δ238U values of adjacent limestone units. We suggest these trends are due to the accumulation of chemically and, more likely, biologically reduced U from anoxic to euxinic bottom water as well as the influence of diagenetic reactions between pore fluids and surrounding sediment and organic matter during diagenesis and catagenesis.

Background reduction in 236U/238U measurements

NASA Astrophysics Data System (ADS)

Buompane, Raffaele; De Cesare, Mario; De Cesare, Nicola; Di Leva, Antonino; D'Onofrio, Antonio; Fifield, L. Keith; Fröhlich, Michaela; Gialanella, Lucio; Marzaioli, Fabio; Sabbarese, Carlo; Terrasi, Filippo; Tims, Stephen; Wallner, Anton

2015-10-01

The measurements of actinide isotopic ratios, in particular 236U/238U, in environmental samples requires high sensitivity. In particular, special effort must be devoted to the suppression of interfering nuclides, such as 235,238U, when measuring 236U. At the AMS facility of CIRCE, isotopic ratios down to ∼10-10 are currently measured using a gas E - ΔE detector. In order to push this limit lower towards natural levels, a time-of-flight system is used, featuring a micro-channel plate start detector and a Si stop detector. As the mass resolution of the latter is limited by the layout, an attempt to reduce the abundant isotope interference by other means has been undertaken. In this study, we report preliminary results on the characterization of the presence of molecular interferences when using UO-, UC- and UC2- as injected molecular ions. In particular the possibility to stabilize the current yield from carbide cathodes has been investigated: it was found that the best cathode preparation procedure is obtained pressing U salts baked at 800 °C mixed with graphite and Al powder. Moreover, the 238U background in 236U measurements is strongly reduced injecting UC- ions, as verified using a time-of-flight detection system. On the other hand, 235U interference is larger with respect to UO- injection, but this increase is smaller than expected on the basis of abundances of 13C and 17O in UC and UC2 molecules on one side and UO, on the other.

Geochemistry of uranium and thorium and natural radioactivity levels of the western Anatolian plutons, Turkey

NASA Astrophysics Data System (ADS)

Papadopoulos, Argyrios; Altunkaynak, Şafak; Koroneos, Antonios; Ünal, Alp; Kamaci, Ömer

2017-10-01

Seventy samples from major plutons (mainly granitic) of Western Anatolia (Turkey) have been analyzed by γ-ray spectrometry to determine the specific activities of 238U, 226Ra, 232Th and 40K (Bq/kg). Τhe natural radioactivity ranged up to 264 Bq/kg for 238U, 229.62 Bq/kg for 226Ra, up to 207.32 Bq/kg for 232Th and up to 2541.95 Bq/kg for 40K. Any possible relationship between the specific activities of 226Ra, 238U, 232Th and 40K and some characteristics of the studied samples (age, rock-type, colour, grain size, occurrence, chemical and mineralogical composition) was investigated. Age, major and trace element geochemistry, color, pluton location and mineralogical composition are likely to affect the concentrations of the measured radionuclides. The range of the Th/U ratio was large (0.003-11.374). The latter, along with 226Ra/238U radioactive secular disequilibrium, is also discussed and explained by magmatic processes during differentiation.

Feasibility of Colliding-beam fast-fission reactor via 238U80++238 U80+ --> 4 FF + 5n + 430 MeV beam with suppressed plutonium and direct conversion of fission fragment (FF) energy into electricity and/or Rocket propellant with high specific impulse

NASA Astrophysics Data System (ADS)

Maglich, Bogdan; Hester, Tim; Calsec Collaboration

2015-10-01

Uranium-uranium colliding beam experiment1, used fully ionized 238U92+ at energy 100GeV --> <-- 100 GeV, has measured total σ = 487 b. Reaction rate of colliding beams is proportional to neutron flux-squared. First functional Auto-Collider3-6, a compact Migma IV, 1 m in diameter, had self-colliding deuterons, D+, of 725 KeV --> <-- 725 KeV, resulting in copious production of T and 3He. U +U Autocollider``EXYDER'' will use strong-focusing magnet7, which would increase reaction rate by 104. 80 times ionized U ions accelerated through 3 MV accelerator, will collide beam 240 MeV --> <-- 240 MeV. Reaction is: 238U80+ +238 U80+ --> 4 FF + 5n + 430 MeV. Using a simple model1 fission σf ~ 100 b. Suppression of Pu by a factor of 106 will be achieved because NO thermal neutron fission can take place; only fast, 1-3 MeV, where σabs is negligible. Direct conversion of 95% of 430 MeV produced is carried by electrically charged FFs which are magnetically funneled for direct conversion of energy of FFs via electrostatic decelerators4,11. 90% of 930 MeV is electrically recoverable. Depending on the assumptions, we project electric _ power density production of 20 to 200 MWe m-3, equivalent to Thermal 1.3 - 13 GWthm-3. If one-half of unburned U is used for propulsion while rest powers system, heavy FF ion mass provides specific impulse Isp = 106 sec., 103 times higher than current rocket engines.

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

NASA Astrophysics Data System (ADS)

Duke, Dana; TKE Team

2014-09-01

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

Natural or fertilizer-derived uranium in irrigation drainage: A case study in southeastern Colorado, U.S.A.

USGS Publications Warehouse

Zielinski, R.A.; Asher-Bolinder, S.; Meier, A.L.; Johnson, C.A.; Szabo, B. J.

1997-01-01

Drainage from heavily cultivated soils may be contaminated with U that is leached from the soil or added as a trace constituent of PO4-based commercial fertilizer. The effect of decades-long application of U-rich fertilizer on the U concentration of irrigation drainage was investigated in a small (14.2 km2) drainage basin in southeastern Colorado. The basin was chosen because previous reports indicated locally anomalous concentrations of dissolved NO3(6-36 mg l-1) and dissolved U (61 ??g l-1) at the mouth of the only stream. Results of this study indicated minimal impact of fertilizer-U compared to natural U leached from the local soils. Detailed sampling of the stream along a 6 mile (9.7 km) reach through heavily cultivated lands indicated marked decoupling of the buildup of dissolved NO3 and U. Dissolved U increased markedly in the upstream half of the reach and correlated positively with increases in Na, Mg, SO4, B and Li derived from leaching of surrounding shaley soils. In contrast, major increases in dissolved NO3 occurred farther downstream where stream water was heavily impacted by ground water return from extensively fertilized fields. Nitrogen isotopic measurements confirmed that dissolved NO3 originated from fertilizer and soil organic N (crop waste). Uranium isotopic measurements of variably uraniferous waters showed little evidence of contamination with fertilizer-derived U of isotopically distinct 234U/238U alpha activity ratio (A.R. = 1.0). Leaching experiments using local alkaline soil, irrigation water and U-rich fertilizer confirmed the ready leachability of soil-bound U and the comparative immobility of U added with liquid fertilizer. Relatively insoluble precipitates containing Ca-P-U were formed by mixing liquid fertilizer with water containing abundant dissolved Ca. In the local soils soluble Ca is provided by dissolution of abundant gypsum. Similar studies are needed elsewhere because the mobility of fertilizer-derived U is dependent on fertilizer type, porewater chemistry and soil properties (pH, moisture, mineralogy, texture).

U-series ages of solitary corals from the California coast by mass spectrometry

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

1991-12-01

The purpose of this study is to evaluate the feasibility of dating fossil solitary corals from Pleistocene marine strandlines outside tropical latitudes using the recently developed high sensitivity, high-precision U-series technique based on thermal-ionization mass-spectrometry (TIMS). The TIMS technique is much more efficient than conventional {alpha} spectrometry and, as a result, multiple samples of an individual coral skeleton, or different specimens from the same bed can be analyzed. Detached and well-rounded fossil specimens of the solitary coral Balanophyllia elegans were collected from relict littoral deposits on emergent marine terraces along the California coast at Cayucos terrace, Shell Beach terrace, Nestormore » terrace, San Diego, Bird Rock terrace, San Diego. Attached living specimens were collected from the intertidal zone on the modern terrace at Moss Beach. The calculated initial {sup 234}U activities in the fossil specimens of Balanophyllia elegans are higher than the {sup 234}U activity in modern seawater or in the modern specimen. The higher initial activities could possibly reflect the influx of {sup 234}U-enriched continental water into Pleistocene coastal waters, or it could reflect the influx of {sup 234}U-enriched continental water into Pleistocene coastal waters, or it could reflect minor diagenetic alteration, a persistent and fundamental problem in dating all corals.« less

Transfer of (40)K, (238)U, (210)Pb, and (210)Po from soil to plant in various locations in south of Syria.

PubMed

Al-Masri, M S; Al-Akel, B; Nashawani, A; Amin, Y; Khalifa, K H; Al-Ain, F

2008-02-01

Transfer factors of (40)K, (238)U, (210)Pb, and (210)Po from soil to some agriculture crops in various locations in south of Syria (Dara'a and Assuwaydaa districts) have been determined. Soil and vegetable crops (green pepper, cucumber, tomato, and eggplant), legumes crops (lentil, chickpea, and broad bean), fruit trees (apple, grape, and olives) and cereals (barley and wheat) were collected and analyzed for (238)U, (210)Pb, and (210)Po. The results have shown that higher transfer factors (calculated as Bqkg(-1) dry wt. plant material per Bqkg(-1) dry wt. soil) for (210)Po, (210)Pb and (238)U were observed in vegetable leaves than fruits and cereals leaves; the highest values of transfer factor (TF) for (238)U were found to be 0.1 for straw of chickpea. Transfer factors for (210)Po varied between 2.8x10(-2) and 2 in fruits of eggplant and grain of barley, respectively. In addition, several parameters affecting transfer factors of the radionuclides were evaluated. The results can be considered as base values for TF of natural radionuclides in the region.

Analysis of plutonium isotope ratios including 238Pu/239Pu in individual U-Pu mixed oxide particles by means of a combination of alpha spectrometry and ICP-MS.

PubMed

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

2017-04-01

Isotope ratio analysis of individual uranium-plutonium (U-Pu) mixed oxide particles contained within environmental samples taken from nuclear facilities is proving to be increasingly important in the field of nuclear safeguards. However, isobaric interferences, such as 238 U with 238 Pu and 241 Am with 241 Pu, make it difficult to determine plutonium isotope ratios in mass spectrometric measurements. In the present study, the isotope ratios of 238 Pu/ 239 Pu, 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the 240 Pu/ 239 Pu, 241 Pu/ 239 Pu, and 242 Pu/ 239 Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of plutonium with UTEVA resins. Furthermore, 238 Pu/ 239 Pu isotope ratios were able to be calculated by using both the 238 Pu/( 239 Pu+ 240 Pu) activity ratios that had been measured through alpha spectrometry and the 240 Pu/ 239 Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including 238 Pu/ 239 Pu, in individual U-Pu mixed oxide particles. Copyright © 2016 Elsevier B.V. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jaffke, Patrick John

This acts as a short note on the effects of varying the value of the endpoints of the thermal, epithermal, and fast flux groups. As expected, varying these endpoints can alter the value of the cross-section for a given nuclide. This effect is quantified in this note for an important nuclide in reactor simulations, 238U. Uranium-238 is responsible for the production of Plutonium in most reactors, making it critical to understand all of the 238U capture modes leading to Plutonium. We explicitly quantify the reaction rates for 238U that are altered when we use a given research reactor fluxmore » and vary the endpoint definitions of said flux as well as the reactor position.« less

Characterization of bauxite residue (red mud) for 235U, 238U, 232Th and 40K using neutron activation analysis and the radiation dose levels as modeled by MCNP.

PubMed

Landsberger, S; Sharp, A; Wang, S; Pontikes, Y; Tkaczyk, A H

2017-07-01

This study employs thermal and epithermal neutron activation analysis (NAA) to quantitatively and specifically determine absorption dose rates to various body parts from uranium, thorium and potassium. Specifically, a case study of bauxite residue (red mud) from an industrial facility was used to demonstrate the feasibility of the NAA approach for radiological safety assessment, using small sample sizes to ascertain the activities of 235 U, 238 U, 232 Th and 40 K. This proof-of-concept was shown to produce reliable results and a similar approach could be used for quantitative assessment of other samples with possible radiological significance. 238 U and 232 Th were determined by epithermal and thermal neutron activation analysis, respectively. 235 U was determined based on the known isotopic ratio of 238 U/ 235 U. 40 K was also determined using epithermal neutron activation analysis to measure total potassium content and then subtracting its isotopic contribution. Furthermore, the work demonstrates the application of Monte Carlo Neutral-Particle (MCNP) simulations to estimate the radiation dose from large quantities of red mud, to assure the safety of humans and the surrounding environment. Phantoms were employed to observe the dose distribution throughout the human body demonstrating radiation effects on each individual organ. Copyright © 2016 Elsevier Ltd. All rights reserved.

Relative intensities of 2. 5 and 14-MeV source neutrons from comparative responses of U-235 and U-238 detectors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jassby, D.L.; Hendel, H.W.; Bosch, H.S.

1988-05-01

The response of polyethylene-moderated U-235 fission counters is only weakly dependent on incident neutron energy, while the response of unmoderated U-238 or Th-232 fission counters increases strongly with energy. A given concentration of D-T neutrons in a mixed DT-DD source results in a unique relative detector response that depends on the parameters R14 and R2.5, where R14 is the ratio of the unmoderated U-238 and moderated U-235 detector efficiencies for a pure 14-MeV neutron source, and R2.5 is the corresponding ratio for a pure 2.5 MeV source. We have determined R14 and R2.5 using D-D and D-T neutron generators insidemore » the TFTR vacuum vessel. The results indicate that, for our detector geometry, the ratio of U-238 to U-235 count rates should increase by a factor of about 3 when the fusion neutron source changes from pure D-D to pure D-T. This calibration is being applied to recent TFTR /open quotes/supershot/close quotes/ data, where the uncollided neutron flux in the post-beam phase contains a high proportion of D-T neutrons from the burnup of D-D tritons. 8 refs., 4 figs,. 2 tabs.« less

Soil-to-cassava transfer of naturally occurring radionuclides from communities along Ghana's oil and gas rich Tano Basin.

PubMed

Doyi, Israel Nutifafa Yawo; Essumang, David Kofi; Agyapong, Asare Kwaku; Asumadu-Sarkodie, Samuel

2018-02-01

Soil-to-plant transfer factor (TF) is widely used to assess the impact of soil radioactivity on agricultural crops. The root crop cassava (Manihot esculenta) provides 30%-50% of the calories consumed in Sub-Saharan Africa and is widely used in South America. γ-ray analysis was used to measure activity concentrations of 238 U, 232 Th, and 40 K in cassava root and soil. The TF values for 238 U, 232 Th, and 40 K were in the range 0.06-0.12, 0.01-0.10 and 0.04-0.28 respectively. The median transfer factors were 0.10 ( 238 U), 0.04 ( 232 Th) and 0.08 ( 40 K). For 238 U and 232 Th, the highest TF values were 0.12 and 0.10 respectively. Copyright © 2017 Elsevier Ltd. All rights reserved.

Uranium biogeochemistry across the redox transition zone of a permanently stratified fjord: Framvaren, Norway

USGS Publications Warehouse

Swarzenski, P.W.; McKee, B.A.; Skei, J.M.; Todd, J.F.

1999-01-01

During August 1995, the vertical concentration profile of dissolved and particulate uranium exhibited strong non-conservative characteristics in the upper 30 m of Framvaren Fjord. There was a pronounced peak in both particulate (> 0.2 ??m; 1.09 nM) and dissolved (< 0.2 ??m; 17.06 nM) uranium in the finely stratified waters at the O2/H2S interface which is positioned well within the euphotic zone at about 20-21 m. Such concentration maxima at the redox boundary are also observed for dissolved organic carbon (DEC), Sr and Ba. Dissolved U levels seen in the water column from 18 m down to 30 m exceeded the high salinity (salinity = 35) U concentrations (13.63 ?? 0.84 nM; Chen, J.H., Edwards, R.L., Wasserburg, G.L., 1986. 238U, 234U and 232Th in seawater. Earth Planet Sci. Lett. 80, 241-251.) observed uniformly in the open ocean. A prolific population of S microbes (e.g., Chromatium, Chlorobium sp.) flourishes at the O2/H2S interface. The source of elevated U at the redox boundary must be due to microbial uptake and subsequent release processes rather than dilution from oceanic uranium. Uranium oxidation state determinations in waters from 1, 22 and 30 m depth reveal that reduced U(IV) is not present in significant abundance, and that the chemical and/or biological reduction of hexavalent uranium is largely inhibited. Our results suggest that U and other trace constituents such as DOC, Sr, Ba, Fe(II), Mn(II) are greatly modified by direct and indirect microbial transformation reactions which are most concentrated across the redox transition zone in Framvaren Fjord.

Activity measurements of a suite of radionuclides (241Am, 239,240Pu, 238Pu, 238U, 234U, 235U, 232Th, 230Th, 228Th, 228Ra, 137Cs, 210Pb, 90Sr and 40K) in biota reference material (Ocean Shellfish): CCRI(II)-S3

NASA Astrophysics Data System (ADS)

Nour, S.; Karam, L. R.; Inn, K. G. W.

2012-01-01

In 2005, the CCRI decided that a comparison undertaken from 2002 to 2008 by the NIST (under the auspices of the Inter-America Metrology System [SIM]) in the development of a new biota (Ocean Shellfish) standard reference material (SRM) was sufficiently well constructed that it could be converted into a supplementary comparison under CCRI(II), with comparison identifier CCRI(II)-S3. This would enable the comparison to be used to support calibration and measurement capability (CMC) claims for radionuclide measurements in reference materials (specifically, animal-based organic materials). Previous comparisons of radionuclides have been of single or multiple nuclides in non-complex matrices and results of such could not be extended to support capabilities to measure the same nuclides in reference materials. The results of this comparison have been used to determine the certified reference value of the SRM. The key comparison working group (KCWG) of the CCRI(II) has approved this approach as a mechanism to link all the results to certified 'reference values' in lieu of the key comparison reference value (KCRV) of these specified radionuclides in this type of matrix (shellfish) so as to support CMCs of similar materials submitted by the present participants. Main text. To reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/. The final report has been peer-reviewed and approved for publication by the CCRI, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Environmental evolution records reflected by radionuclides in the sediment of coastal wetlands: A case study in the Yellow River Estuary wetland.

PubMed

Wang, Qidong; Song, Jinming; Li, Xuegang; Yuan, Huamao; Li, Ning; Cao, Lei

2016-10-01

Vertical profiles of environmental radionuclides ( 210 Pb, 137 Cs, 238 U, 232 Th, 226 Ra and 4 0 K) in a sediment core (Y1) of the Yellow River Estuary wetland were investigated to assess whether environmental evolutions in the coastal wetland could be recorded by the distributions of radionuclides. Based on 210 Pb and 137 Cs dating, the average sedimentation rate of core Y1 was estimated to be 1.0 cm y -1 . Vertical distributions of natural radionuclides ( 238 U, 232 Th, 226 Ra and 40 K) changed dramatically, reflecting great changes in sediment input. Concentrations of 238 U, 232 Th, 226 Ra and 40 K all had significant positive relationships with organic matter and clay content, but their distributions were determined by different factors. Factor analysis showed that 238 U was determined by the river sediment input while 226 Ra was mainly affected by the seawater erosion. Environmental changes such as river channel migrations and sediment discharge variations could always cause changes in the concentrations of radionuclides. High concentrations of 238 U and 226 Ra were consistent with high accretion rate. Frequent seawater intrusion decreased the concentration of 226 Ra significantly. The value of 238 U/ 226 Ra tended to be higher when the sedimentation rate was low and tide intrusion was frequent. In summary, environmental evolutions in the estuary coastal wetland could be recorded by the vertical profiles of natural radionuclides. Copyright © 2016 Elsevier Ltd. All rights reserved.

Contributions of 18 food categories to intakes of 232Th and 238U in Japan.

PubMed

Shiraishi, K; Tagami, K; Muramastu, Y; Yamamoto, M

2000-01-01

Daily intakes of 232Th and 238U and contributions of food categories to those nuclide intakes in Japanese were estimated using a market basket study for 18 food categories. Food categories having higher 238U contents (per g-fresh) were found to be as follows: seaweeds 1,140 microBq; fishes and shellfishes 37 microBq; nuts and seeds 11 microBq; bean products 8.6 microBq; and cooked meals 7.3 microBq. Big contributors to the daily 238U intake in Japan were as follows: seaweeds (50%); fishes and shellfishes (26%); and bean products (4.3%). For 232Th, higher contents (per g-fresh) were found as follows: seaweeds 28 microBq; fishes and shellfishes 13 microBq; nuts and seeds 8.2 microBq; green vegetables 3.9 microBq; cooked meals 3.5 microBq; and bean products 2.9 microBq. Big contributors to the daily 232Th intake were as follows: fishes and shellfishes (44%); green vegetables (11%); bean products (7.4%); and seaweeds (6.0%). For both nuclides, marine food products were big contributors, while minor contributors were oil and fats, eggs, and cooked meals. Daily intakes of 232Th and 238U in Japan were estimated to be 2.7 mBq and 14 mBq per person from the intakes of the 18 categories, respectively. Annual effective doses were estimated to be 232Th, 2.2 x 10(-7) Sv, and 238U, 2.2 x 10(-7) Sv.

Beta decay heat following U-235, U-238 and Pu-239 neutron fission

NASA Astrophysics Data System (ADS)

Li, Shengjie

1997-09-01

This is an experimental study of beta-particle decay heat from 235U, 239Pu and 238U aggregate fission products over delay times 0.4-40,000 seconds. The experimental results below 2s for 235U and 239Pu, and below 20s for 238U, are the first such results reported. The experiments were conducted at the UMASS Lowell 5.5-MV Van de Graaff accelerator and 1-MW swimming-pool research reactor. Thermalized neutrons from the 7Li(p,n)7Be reaction induced fission in 238U and 239Pu, and fast neutrons produced in the reactor initiated fission in 238U. A helium-jet/tape-transport system rapidly transferred fission fragments from a fission chamber to a low background counting area. Delay times after fission were selected by varying the tape speed or the position of the spray point relative to the beta spectrometer that employed a thin-scintillator-disk gating technique to separate beta-particles from accompanying gamma-rays. Beta and gamma sources were both used in energy calibration. Based on low-energy(<1 MeV) internal-conversion electron studies, a set of trial responses for the spectrometer was established and spanned electron energies 0-10 MeV. Measured beta spectra were unfolded for their energy distributions by the program FERD, and then compared to other measurements and summation calculations based on ENDF/B-VI fission-product data performed on the LANL Cray computer. Measurements of the beta activity as a function of decay time furnished a relative normalization. Results for the beta decay heat are presented and compared with other experimental data and the summation calculations.

Role of colloidal material in the removal of 234Th in the Canada basin of the Arctic Ocean

USGS Publications Warehouse

Baskaran, M.; Swarzenski, P.W.; Porcelli, D.

2003-01-01

The phase partitioning of 234Th between dissolved ( 200m, general equilibrium existed between total 234Th and 238U. The inventory of SPM and the specific activity of particulate 234Th in the Canada Basin was about an order of magnitude higher than the profile reported for the Alpha Ridge ice camp station. This higher concentration of SPM in the southwestern Canada Basin is likely derived from ice-rafted sedimentary particles. Inventories of nutrients, and dissolved organic carbon and nitrogen in the upper 100 m of the Canada Basin are comparable to the other estimates for the central Arctic Ocean. Comparison of the mass concentrations of colloidal and filter-retained particulate matter as well as the activity of 234Th in these phases indicates that only a very small component of the colloidal material is actively involved in Th scavenging. Lower values of the conditional partition coefficient between the colloidal and dissolved phase indicate that the Arctic colloids are less reactive than colloidal material from other regions. The conditional partition coefficient between the filter-retained and dissolved phases (Kf) is generally higher than that for other regions, which is attributed to the higher complexation capacity of glacio-marine sedimentary particles in these waters. The 234Th-derived export of POC for the shelf and deep Canada Basin ranges between 5.6 and 6.5 mmol m-2 d-1, and is in agreement with other estimates reported for the central Arctic Ocean and Beaufort Sea. ?? 2003 Elsevier Ltd. All rights reserved.

Photofission cross-section ratio measurement of 235U/238U using monoenergetic photons in the energy range of 9.0-16.6 MeV

NASA Astrophysics Data System (ADS)

Krishichayan; Bhike, Megha; Finch, S. W.; Howell, C. R.; Tonchev, A. P.; Tornow, W.

2017-05-01

Photofission cross-section ratios of 235U and 238U have been measured using monoenergetic photon beams at the HIγS facility of TUNL. These measurements have been performed in small energy steps between 9.0 and 16.6 MeV using a dual-fission ionization chamber. Measured cross-section ratios are compared with the previous experimental data as well as with the recent evaluated nuclear data library ENDF.

Observations of 231Pa/ 235U disequilibrium in volcanic rocks

NASA Astrophysics Data System (ADS)

Pickett, David A.; Murrell, Michael T.

1997-04-01

We present here the first survey of ( 231Pa/ 235U) ratios in volcanic rocks; such measurements are made possible by new mass spectrometric techniques. The data place new constraints on the timing and extent of magma source and evolutionary processes, particularly due to the sensitivity of the 231Pa- 235U pair and its intermediate time scale ( 231Pat 1/2 = 33 ky). ( 231Pa/ 235U) is found to vary widely, from 0.2 in carbonatites to 1.1-2.9 in basalts and 0.9-2.2 in arcs. Substantial Pa enrichment is nearly ubiquitous, suggestive of the relative incompatibility of Pa, qualitatively consistent with available partitioning data. The level of 231Pa- 235U disequilibrium typically far exceeds that of 230Th- 238U and is comparable to 226Ra- 230Th. The high ( 231Pa/ 235U) ratios in MORB and other basalts reflect a large degree of discrimination between two incompatible elements, posing challenges for modelling of melt generation and migration. Fundamental differences in ( 231Pa/ 235U) among different basaltic environments are likely related to contrasts in melting zone conditions (e.g., melting rate). Strong ( 231Pa/ 235U) disequilibria in continental basalts, for which ( 230Th/ 238U) disequilibria are small or absent, demonstrate that Pa-U fractionation is possible in both garnet and spinel mantle stability fields. In arcs, correlation of ( 231Pa/ 235U) and ( 230Th/ 238U) is consistent with U enrichment via slab-derived fluids, a process which is additional to the still dominant Pa enrichment. An important new constraint is provided by the observation that the near-equilibrium ( 230Th/ 238U) common to arcs and continental basalts is not typically accompanied by near-equilibrium ( 231Pa/ 235U), arguing against the influence of long magma history, crustal material, or equilibrium mantle sources in affecting decay-series ratios. Small sample sets from two silicic centers illustrate: (1) recent, rapid U enrichment in the magma chamber (El Chichón); and (2) the failure of substantial magma H 2O-CO 2 degassing to effect U-Th-Pa fractionation (Mono Craters).

Towards the high-accuracy determination of the 238U fission cross section at the threshold region at CERN - n_TOF

NASA Astrophysics Data System (ADS)

Diakaki, M.; Audouin, L.; Berthoumieux, E.; Calviani, M.; Colonna, N.; Dupont, E.; Duran, I.; Gunsing, F.; Leal-Cidoncha, E.; Le Naour, C.; Leong, L. S.; Mastromarco, M.; Paradela, C.; Tarrio, D.; Tassan-Got, L.; Aerts, G.; Altstadt, S.; Alvarez, H.; Alvarez-Velarde, F.; Andriamonje, S.; Andrzejewski, J.; Badurek, G.; Barbagallo, M.; Baumann, P.; Becares, V.; Becvar, F.; Belloni, F.; Berthier, B.; Billowes, J.; Boccone, V.; Bosnar, D.; Brugger, M.; Calvino, F.; Cano-Ott, D.; Capote, R.; Carrapiço, C.; Cennini, P.; Cerutti, F.; Chiaveri, E.; Chin, M.; Cortes, G.; Cortes-Giraldo, M. A.; Cosentino, L.; Couture, A.; Cox, J.; David, S.; Dillmann, I.; Domingo-Pardo, C.; Dressler, R.; Dridi, W.; Eleftheriadis, C.; Embid-Segura, M.; Ferrant, L.; Ferrari, A.; Finocchiaro, P.; Fraval, K.; Fujii, K.; Furman, W.; Ganesan, S.; Garcia, A. R.; Giubrone, G.; Gomez-Hornillos, M. B.; Goncalves, I. F.; Gonzalez-Romero, E.; Goverdovski, A.; Gramegna, F.; Griesmayer, E.; Guerrero, C.; Gurusamy, P.; Haight, R.; Heil, M.; Heinitz, S.; Igashira, M.; Isaev, S.; Jenkins, D. G.; Jericha, E.; Kadi, Y.; Kaeppeler, F.; Karadimos, D.; Karamanis, D.; Kerveno, M.; Ketlerov, V.; Kivel, N.; Kokkoris, M.; Konovalov, V.; Krticka, M.; Kroll, J.; Lampoudis, C.; Langer, C.; Lederer, C.; Leeb, H.; Lo Meo, S.; Losito, R.; Lozano, M.; Manousos, A.; Marganiec, J.; Martinez, T.; Marrone, S.; Massimi, C.; Mastinu, P.; Mendoza, E.; Mengoni, A.; Milazzo, P. M.; Mingrone, F.; Mirea, M.; Mondelaers, W.; Moreau, C.; Mosconi, M.; Musumarra, A.; O'Brien, S.; Pancin, J.; Patronis, N.; Pavlik, A.; Pavlopoulos, P.; Perkowski, J.; Perrot, L.; Pigni, M. T.; Plag, R.; Plompen, A.; Plukis, L.; Poch, A.; Pretel, C.; Praena, J.; Quesada, J.; Rauscher, T.; Reifarth, R.; Riego, A.; Roman, F.; Rudolf, G.; Rubbia, C.; Rullhusen, P.; Salgado, J.; Santos, C.; Sarchiapone, L.; Sarmento, R.; Saxena, A.; Schillebeeckx, P.; Schmidt, S.; Schumann, D.; Stephan, C.; Tagliente, G.; Tain, J. L.; Tavora, L.; Terlizzi, R.; Tsinganis, A.; Valenta, S.; Vannini, G.; Variale, V.; Vaz, P.; Ventura, A.; Versaci, R.; Vermeulen, M. J.; Villamarin, D.; Vincente, M. C.; Vlachoudis, V.; Vlastou, R.; Voss, F.; Wallner, A.; Walter, S.; Ware, T.; Weigand, M.; Weiß, C.; Wiesher, M.; Wisshak, K.; Wright, T.; Zugec, P.

2016-03-01

The 238U fission cross section is an international standard beyond 2 MeV where the fission plateau starts. However, due to its importance in fission reactors, this cross-section should be very accurately known also in the threshold region below 2 MeV. The 238U fission cross section has been measured relative to the 235U fission cross section at CERN - n_TOF with different detection systems. These datasets have been collected and suitably combined to increase the counting statistics in the threshold region from about 300 keV up to 3 MeV. The results are compared with other experimental data, evaluated libraries, and the IAEA standards.

Fusion and direct reactions around the barrier for the systems {sup 7,9}Be,{sup 7}Li+{sup 238}U

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raabe, R.; Angulo, C.; Charvet, J. L.

2006-10-15

We present new cross section data for the complete fusion of the weakly bound systems {sup 7,9}Be and {sup 7}Li on {sup 238}U at energies around the Coulomb barrier. In the same measurement, yields for direct processes and incomplete fusion are detected. For all systems, a suppression of the complete fusion cross section around and above the barrier is observed. At energies below the barrier, the fusion of the {sup 7}Be+{sup 238}U system shows no enhancement with respect to simple model predictions.

Inelastic neutron scattering from {sup 238}U

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moxon, M.C.; Wartena, J.A.; Weigmann, H.

1994-12-31

A measurement of the neutron inelastic scattering cross-section of {sup 238}U at 4 distant neutron energies in the low keV region has been undertaken using a 30m flight path on the pulsed neutron source GELINA. The scattered neutrons are detected in a plastic scintillator after passing through a 270 mm iron filter. The values obtained for the cross-section to the first excited 2{sup +} state in {sup 238}U are 293{+-}31, 660{+-}296, 978{+-}73 and 1176{+-}95 mb at neutron energies of 68.2, 126.6, 182.4 and 213.6 keV respectively.

Formation and preservation of pedogenic carbonates in South India, links with paleo-monsoon and pedological conditions: Clues from Sr isotopes, U-Th series and REEs

NASA Astrophysics Data System (ADS)

Violette, Aurélie; Riotte, Jean; Braun, Jean-Jacques; Oliva, Priscia; Marechal, Jean-Christophe; Sekhar, M.; Jeandel, Catherine; Subramanian, S.; Prunier, Jonathan; Barbiero, Laurent; Dupre, Bernard

2010-12-01

The influence of the pedogenic and climatic contexts on the formation and preservation of pedogenic carbonates in a climosequence in the Western Ghats (Karnataka Plateau, South West India) has been studied. Along the climosequence, the current mean annual rainfall (MAR) varies within a 80 km transect from 6000 mm at the edge of the Plateau to 500 mm inland. Pedogenic carbonates occur in the MAR range of 500-1200 mm. In the semi-arid zone (MAR: 500-900 mm), carbonates occur (i) as thick hardpan calcretes on pediment slopes and (ii) as nodular horizons in polygenic black soils (i.e. vertisols). In the sub-humid zone (MAR: 900-1500 mm), pedogenic carbonates are disseminated in the black soil matrices either as loose, irregular and friable nodules of millimetric size or as indurated botryoidal nodules of centimetric to pluricentimetric size. They also occur at the top layers of the saprolite either as disseminated pluricentimetric indurated nodules or carbonate-cemented lumps of centimetric to decimetric size. Chemical and isotopic ( 87Sr/ 86Sr) compositions of the carbonate fraction were determined after leaching with 0.25 N HCl. The corresponding residual fractions containing both primary minerals and authigenic clays were digested separately and analyzed. The trend defined by the 87Sr/ 86Sr signatures of both labile carbonate fractions and corresponding residual fractions indicates that a part of the labile carbonate fraction is genetically linked to the local soil composition. Considering the residual fraction of each sample as the most likely lithogenic source of Ca in carbonates, it is estimated that from 24% to 82% (55% on average) of Ca is derived from local bedrock weathering, leading to a consumption of an equivalent proportion of atmospheric CO 2. These values indicate that climatic conditions were humid enough to allow silicate weathering: MAR at the time of carbonate formation likely ranged from 400 to 700 mm, which is 2- to 3-fold less than the current MAR at these locations. The Sr, U and Mg contents and the ( 234U/ 238U) activity ratio in the labile carbonate fraction help to understand the conditions of carbonate formation. The relatively high concentrations of Sr, U and Mg in black soil carbonates may indicate fast growth and accumulation compared to carbonates in saprolite, possibly due to a better confinement of the pore waters which is supported by their high ( 234U/ 238U) signatures, and/or to higher content of dissolved carbonates in the pore waters. The occurrence of Ce, Mn and Fe oxides in the cracks of carbonate reflects the existence of relatively humid periods after carbonate formation. The carbonate ages determined by the U-Th method range from 1.33 ± 0.84 kyr to 7.5 ± 2.7 kyr and to a cluster of five ages around 20 kyr, i.e. the Last Glacial Maximum period. The young occurrences are only located in the black soils, which therefore constitute sensitive environments for trapping and retaining atmospheric CO 2 even on short time scales. The maximum age of carbonates depends on their location in the climatic gradient: from about 20 kyr for centimetric nodules at Mule Hole (MAR = 1100 mm/yr) to 200 kyr for the calcrete at Gundlupet (MAR = 700 mm/yr, Durand et al., 2007). The intensity of rainfall during wet periods would indeed control the lifetime of pedogenic carbonates and thus the duration of inorganic carbon storage in soils.

Room temperature electrodeposition of actinides from ionic solutions

DOEpatents

Hatchett, David W.; Czerwinski, Kenneth R.; Droessler, Janelle; Kinyanjui, John

2017-04-25

Uranic and transuranic metals and metal oxides are first dissolved in ozone compositions. The resulting solution in ozone can be further dissolved in ionic liquids to form a second solution. The metals in the second solution are then electrochemically deposited from the second solutions as room temperature ionic liquid (RTIL), tri-methyl-n-butyl ammonium n-bis(trifluoromethansulfonylimide) [Me.sub.3N.sup.nBu][TFSI] providing an alternative non-aqueous system for the extraction and reclamation of actinides from reprocessed fuel materials. Deposition of U metal is achieved using TFSI complexes of U(III) and U(IV) containing the anion common to the RTIL. TFSI complexes of uranium were produced to ensure solubility of the species in the ionic liquid. The methods provide a first measure of the thermodynamic properties of U metal deposition using Uranium complexes with different oxidation states from RTIL solution at room temperature.

Evaluation of naturally occurring radioactivity across the State of Kuwait using high-resolution gamma-ray spectrometry

NASA Astrophysics Data System (ADS)

Bajoga, A. D.; Alazemi, N.; Shams, H.; Regan, P. H.; Bradley, D. A.

2017-08-01

A study of natural radioactivity from 90 different soil samples from the state of Kuwait has been carried out to ascertain the NORM concentration values across the country. The calculated activity concentrations were determined from: (i) the decays of the 226Ra, 214Pb and 214Bi members of the 4n+2 decay chain headed by 238U and; (ii) the 228Ac, 212Pb and 208Tl members of the 4n chain headed by 232Th. The study also included evaluations for the 235U decay chain with the 186 keV doublet transition used together with the measured 4n+2 activity concentration values to determine the 235U/238U isotopic ratios for each sample. The values for the arithmetic mean activity concentrations for 90 separate locations across Kuwait as determined in the current work were 17.2, 14.1, and 368 Bq/kg, with standard deviations of 5.2, 3.7 and 90 Bq/kg for the 238U, 232Th and 40K activity concentrations respectively. Measured isotope ratios for 235U/238U give an arithmetic mean value for all of the samples of 0.045±0.003, consistent with that expected for natural uranium. These results indicate no evidence for a radiologically significant dispersion of additional depleted uranium across the entire State of Kuwait from the 1991 Gulf War.

Experimental determination of U and Th partitioning between clinopyroxene and natural and synthetic basaltic liquid

NASA Technical Reports Server (NTRS)

Latourrette, T. Z.; Burnett, D. S.

1992-01-01

Experimental measurements of U and the partition coefficients between clinopyroxene and synthetic and natural basaltic liquid are presented. The results demonstrate that crystal-liquid U-Th fractionation is fO2-dependent and that U in terrestrial magmas is not entirely tetravalent. During partial melting, the liquid will have a Th/U ratio less than the clinopyroxene in the source. The observed U-238 - Th-230 disequilibrium in MORB requires that the partial melt should have a U/Th ratio greater than the bulk source and therefore cannot result from clinopyroxene-liquid partitioning. Further, the magnitudes of the measured partition coefficients are too small to generate significant U-Th fractionation in either direction. Assuming that clinopyroxene contains the bulk of the U and Th in the MORB source, the results indicate that U-238 - Th-230 disequilibrium in MORB may not be caused by partial melting at all.

A new method to measure the U-235 content in fresh LWR fuel assemblies via fast-neutron passive self-interrogation

DOE PAGES

Menlove, Howard Olsen; Belian, Anthony P.; Geist, William H.; ...

2017-10-07

The purpose of this paper is to provide a solution to a decades old safeguards problem in the verification of the fissile concentration in fresh light water reactor (LWR) fuel assemblies. The problem is that the burnable poison (e.g. Gd 2O 3) addition to the fuel rods decreases the active neutron assay for the fuel assemblies. This paper presents a new innovative method for the verification of the 235U linear mass density in fresh LEU fuel assemblies that is insensitive to the burnable poison content. The technique makes use of the 238U atoms in the fuel rods to self-interrogate themore » 235U mass. The innovation for the new approach is that the 238U spontaneous fission (SF) neutrons from the rods induces fission reactions (IF) in the 235U that are time correlated with the SF source neutrons. Thus, the coincidence gate counting rate benefits from both the nu-bar of the 238U SF (2.07) and the 235U IF (2.44) for a fraction of the IF reactions. Whereas, the 238U SF background has no time-correlation boost. The higher the detection efficiency, the higher the correlated boost because background neutron counts from the SF are being converted to signal doubles. This time-correlation in the IF signal increases signal/background ratio that provides a good precision for the net signal from the 235U mass. The hard neutron energy spectrum makes the technique insensitive to the burnable poison loading where a Cd or Gd liner on the detector walls is used to prevent thermal-neutron reflection back into the fuel assembly from the detector. Here, we have named the system the fast-neutron passive collar (FNPC).« less

Determination of depleted uranium in urine via isotope ratio measurements using large-bore direct injection high efficiency nebulizer-inductively coupled plasma mass spectrometry.

PubMed

Westphal, Craig S; McLean, John A; Hakspiel, Shelly J; Jackson, William E; McClain, David E; Montaser, Akbar

2004-09-01

Inductively coupled plasma mass spectrometry (ICP-MS), coupled with a large-bore direct injection high efficiency nebulizer (LB-DIHEN), was utilized to determine the concentration and isotopic ratio of uranium in 11 samples of synthetic urine spiked with varying concentrations and ratios of uranium isotopes. Total U concentrations and (235)U/(238)U isotopic ratios ranged from 0.1 to 10 microg/L and 0.0011 and 0.00725, respectively. The results are compared with data from other laboratories that used either alpha-spectrometry or quadrupole-based ICP-MS with a conventional nebulizer-spray chamber arrangement. Severe matrix effects due to the high total dissolved solid content of the samples resulted in a 60 to 80% loss of signal intensity, but were compensated for by using (233)U as an internal standard. Accurate results were obtained with LB-DIHEN-ICP-MS, allowing for the positive identification of depleted uranium based on the (235)U/(238)U ratio. Precision for the (235)U/(238)U ratio is typically better than 5% and 15% for ICP-MS and alpha-spectrometry, respectively, determined over the concentrations and ratios investigated in this study, with the LB-DIHEN-ICP-MS system providing the most accurate results. Short-term precision (6 min) for the individual (235)U and (238)U isotopes in synthetic urine is better than 2% (N = 7), compared to approximately 5% for conventional nebulizer-spray chamber arrangements and >10% for alpha-spectrometry. The significance of these measurements is discussed for uranium exposure assessment of Persian Gulf War veterans affected by depleted uranium ammunitions.

A new method to measure the U-235 content in fresh LWR fuel assemblies via fast-neutron passive self-interrogation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Menlove, Howard Olsen; Belian, Anthony P.; Geist, William H.

The purpose of this paper is to provide a solution to a decades old safeguards problem in the verification of the fissile concentration in fresh light water reactor (LWR) fuel assemblies. The problem is that the burnable poison (e.g. Gd 2O 3) addition to the fuel rods decreases the active neutron assay for the fuel assemblies. This paper presents a new innovative method for the verification of the 235U linear mass density in fresh LEU fuel assemblies that is insensitive to the burnable poison content. The technique makes use of the 238U atoms in the fuel rods to self-interrogate themore » 235U mass. The innovation for the new approach is that the 238U spontaneous fission (SF) neutrons from the rods induces fission reactions (IF) in the 235U that are time correlated with the SF source neutrons. Thus, the coincidence gate counting rate benefits from both the nu-bar of the 238U SF (2.07) and the 235U IF (2.44) for a fraction of the IF reactions. Whereas, the 238U SF background has no time-correlation boost. The higher the detection efficiency, the higher the correlated boost because background neutron counts from the SF are being converted to signal doubles. This time-correlation in the IF signal increases signal/background ratio that provides a good precision for the net signal from the 235U mass. The hard neutron energy spectrum makes the technique insensitive to the burnable poison loading where a Cd or Gd liner on the detector walls is used to prevent thermal-neutron reflection back into the fuel assembly from the detector. Here, we have named the system the fast-neutron passive collar (FNPC).« less

A new method to measure the U-235 content in fresh LWR fuel assemblies via fast-neutron passive self-interrogation

NASA Astrophysics Data System (ADS)

Menlove, Howard; Belian, Anthony; Geist, William; Rael, Carlos

2018-01-01

The purpose of this paper is to provide a solution to a decades old safeguards problem in the verification of the fissile concentration in fresh light water reactor (LWR) fuel assemblies. The problem is that the burnable poison (e.g. Gd2O3) addition to the fuel rods decreases the active neutron assay for the fuel assemblies. This paper presents a new innovative method for the verification of the 235U linear mass density in fresh LEU fuel assemblies that is insensitive to the burnable poison content. The technique makes use of the 238U atoms in the fuel rods to self-interrogate the 235U mass. The innovation for the new approach is that the 238U spontaneous fission (SF) neutrons from the rods induces fission reactions (IF) in the 235U that are time correlated with the SF source neutrons. Thus, the coincidence gate counting rate benefits from both the nu-bar of the 238U SF (2.07) and the 235U IF (2.44) for a fraction of the IF reactions. Whereas, the 238U SF background has no time-correlation boost. The higher the detection efficiency, the higher the correlated boost because background neutron counts from the SF are being converted to signal doubles. This time-correlation in the IF signal increases signal/background ratio that provides a good precision for the net signal from the 235U mass. The hard neutron energy spectrum makes the technique insensitive to the burnable poison loading where a Cd or Gd liner on the detector walls is used to prevent thermal-neutron reflection back into the fuel assembly from the detector. We have named the system the fast-neutron passive collar (FNPC).

Evaluation strategies for isotope ratio measurements of single particles by LA-MC-ICPMS.

PubMed

Kappel, S; Boulyga, S F; Dorta, L; Günther, D; Hattendorf, B; Koffler, D; Laaha, G; Leisch, F; Prohaska, T

2013-03-01

Data evaluation is a crucial step when it comes to the determination of accurate and precise isotope ratios computed from transient signals measured by multi-collector-inductively coupled plasma mass spectrometry (MC-ICPMS) coupled to, for example, laser ablation (LA). In the present study, the applicability of different data evaluation strategies (i.e. 'point-by-point', 'integration' and 'linear regression slope' method) for the computation of (235)U/(238)U isotope ratios measured in single particles by LA-MC-ICPMS was investigated. The analyzed uranium oxide particles (i.e. 9073-01-B, CRM U010 and NUSIMEP-7 test samples), having sizes down to the sub-micrometre range, are certified with respect to their (235)U/(238)U isotopic signature, which enabled evaluation of the applied strategies with respect to precision and accuracy. The different strategies were also compared with respect to their expanded uncertainties. Even though the 'point-by-point' method proved to be superior, the other methods are advantageous, as they take weighted signal intensities into account. For the first time, the use of a 'finite mixture model' is presented for the determination of an unknown number of different U isotopic compositions of single particles present on the same planchet. The model uses an algorithm that determines the number of isotopic signatures by attributing individual data points to computed clusters. The (235)U/(238)U isotope ratios are then determined by means of the slopes of linear regressions estimated for each cluster. The model was successfully applied for the accurate determination of different (235)U/(238)U isotope ratios of particles deposited on the NUSIMEP-7 test samples.

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.

Environmental 238U and 232Th concentration measurements in an area of high level natural background radiation at Palong, Johor, Malaysia.

PubMed

Ramli, A Termizi; Hussein, A Wahab M A; Wood, A Khalik

2005-01-01

Concentrations of uranium-238 and thorium-232 in soil, water, grass, moss and oil-palm fruit samples collected from an area of high background radiation were determined using neutron activation analysis (NAA). U-238 concentration in soil ranged from 4.9 mg kg(-1) (58.8 Bq kg(-1)) to 40.4 mg kg(-1) (484.8 Bq kg(-1)), Th-232 concentration ranged from 14.9 mg kg(-1) (59.6 Bq kg(-1)) to 301.0 mg kg(-1) (1204 Bq kg(-1)). The concentration of U-238 in grass samples ranged from below the detection limit to 0.076 mg kg(-1) (912 mBq kg(-1)), and Th-232 ranged from 0.008 mg kg(-1) (32 mBq kg(-1)) to 0.343 mg kg(-1) (1.372 Bq kg(-1)). U-238 content in water samples ranged from 0.33 mg kg(-1) (4.0 Bq L(-1)) to 1.40 mg kg(-1) (16.8 Bq L(-1)), and Th-232 ranged from 0.19 mg kg(-1) (0.76 Bq L(-1)) to 0.66 mg kg(-1) (2.64 Bq L(-1)). It can be said that the concentrations of environmental U-238 and Th-232 in grass and water samples in the study area are insignificant. Mosses were found to be possible bio-radiological indicators due to their high absorption of the heavy radioelements from the environment.

Estimation of dose delivered to accelerator devices from stripping of 18.5 MeV/n 238U ions using the FLUKA code

NASA Astrophysics Data System (ADS)

Oranj, Leila Mokhtari; Lee, Hee-Seock; Leitner, Mario Santana

2017-12-01

In Korea, a heavy ion accelerator facility (RAON) has been designed for production of rare isotopes. The 90° bending section of this accelerator includes a 1.3- μm-carbon stripper followed by two dipole magnets and other devices. An incident beam is 18.5 MeV/n 238U33+,34+ ions passing through the carbon stripper at the beginning of the section. The two dipoles are tuned to transport 238U ions with specific charge states of 77+, 78+, 79+, 80+ and 81+. Then other ions will be deflected at the bends and cause beam losses. These beam losses are a concern to the devices of transport/beam line. The absorbed dose in devices and prompt dose in the tunnel were calculated using the FLUKA code in order to estimate radiation damage of such devices located at the 90° bending section and for the radiation protection. A novel method to transport multi-charged 238U ions beam was applied in the FLUKA code by using charge distribution of 238U ions after the stripper obtained from LISE++ code. The calculated results showed that the absorbed dose in the devices is influenced by the geometrical arrangement. The maximum dose was observed at the coils of first, second, fourth and fifth quadruples placed after first dipole magnet. The integrated doses for 30 years of operation with 9.5 p μA 238U ions were about 2 MGy for those quadrupoles. In conclusion, the protection of devices particularly, quadruples would be necessary to reduce the damage to devices. Moreover, results showed that the prompt radiation penetrated within the first 60 - 120 cm of concrete.

Mid-ocean ridge basalt generation along the slow-spreading, South Mid-Atlantic Ridge (5-11°S): Inferences from 238U-230Th-226Ra disequilibria

NASA Astrophysics Data System (ADS)

Turner, Simon; Kokfelt, Thomas; Hauff, Folkmar; Haase, Karsten; Lundstrom, Craig; Hoernle, Kaj; Yeo, Isobel; Devey, Colin

2015-11-01

U-series disequilibria have provided important constraints on the physical processes of partial melting that produce basaltic magma beneath mid-ocean ridges. Here we present the first 238U-230Th-226Ra isotope data for a suite of 83 basalts sampled between 5°S and 11°S along the South Mid-Atlantic Ridge. This section of the ridge can be divided into 5 segments (A0-A4) and the depths to the ridge axis span much of the global range, varying from 1429 to 4514 m. Previous work has also demonstrated that strong trace element and radiogenic isotope heterogeneity existed in the source regions of these basalts. Accordingly, this area provides an ideal location in which to investigate the effects of both inferred melt column length and recycled materials. 226Ra-230Th disequilibria indicate that the majority of the basalts are less than a few millennia old such that their 230Th values do not require any age correction. The U-Th isotope data span a significant range from secular equilibrium up to 32% 230Th excess, also similar to the global range, and vary from segment to segment. However, the (230Th/238U) ratios are not negatively correlated with axial depth and the samples with the largest 230Th excesses come from the deepest ridge segment (A1). Two sub-parallel and positively sloped arrays (for segments A0-2 and A3 and A4) between (230Th/238U) and Th/U ratios can be modelled in various ways as mixing between melts from peridotite and recycled mafic lithologies. Despite abundant evidence for source heterogeneity, there is no simple correlation between (230Th/238U) and radiogenic isotope ratios suggesting that at least some of the trace element and radiogenic isotope variability may have been imparted to the source regions >350 kyr prior to partial melting to produce the basalts. In our preferred model, the two (230Th/238U) versus Th/U arrays can be explained by mixing of melts from one or more recycled mafic lithologies with melts derived from chemically heterogeneous peridotite source regions.

Uncertainty analysis on reactivity and discharged inventory for a pressurized water reactor fuel assembly due to {sup 235,238}U nuclear data uncertainties

DOE Office of Scientific and Technical Information (OSTI.GOV)

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

2012-07-01

This paper discusses the uncertainty analysis on reactivity and inventory for a typical PWR fuel element as a result of uncertainties in {sup 235,238}U nuclear data. A typical Westinghouse 3-loop fuel assembly fuelled with UO{sub 2} fuel with 4.8% enrichment has been selected. The Total Monte-Carlo method has been applied using the deterministic transport code DRAGON. This code allows the generation of the few-groups nuclear data libraries by directly using data contained in the nuclear data evaluation files. The nuclear data used in this study is from the JEFF3.1 evaluation, and the nuclear data files for {sup 238}U and {supmore » 235}U (randomized for the generation of the various DRAGON libraries) are taken from the nuclear data library TENDL. The total uncertainty (obtained by randomizing all {sup 238}U and {sup 235}U nuclear data in the ENDF files) on the reactor parameters has been split into different components (different nuclear reaction channels). Results show that the TMC method in combination with a deterministic transport code constitutes a powerful tool for performing uncertainty and sensitivity analysis of reactor physics parameters. (authors)« less

A Signature Distinguishing Fissile From Non-Fissile Materials Using Linearly Polarized Gamma Rays

NASA Astrophysics Data System (ADS)

Mueller, J. M.; Ahmed, M. W.; Karwowski, H. J.; Myers, L. S.; Sikora, M. H.; Stave, S.; Tompkins, J. R.; Zimmerman, W. R.; Weller, H. R.

2013-04-01

Photofission of ^233,235,238U, ^239,240Pu, and ^232Th was induced by nearly 100% linearly polarized, high intensity (˜10^7 γs per second), and nearly-monoenergetic γ-ray beams of energies between 5.6 and 7.3 MeV at the High Intensity γ-ray Source (HIγS). An array of 18 liquid scintillating detectors was used to measure prompt fission neutron angular distributions. The ratio of prompt fission neutron yields parallel to the plane of beam polarization to the yields perpendicular to this plane was measured as a function of beam and neutron energy, as described in a recent publication showing results from ^235,238U, ^239Pu, and ^232Th [1]. A ratio near unity was found for ^233,235U and ^239Pu while a significant ratio (˜1.5-3) was found for ^238U, ^240Pu, and ^232Th. This large difference could be used to distinguish fissile isotopes (such as ^233,235U and ^239Pu) from non-fissile isotopes (such as ^238U, ^240Pu, and ^232Th). Polarization ratios as a function of the relative abundance of fissile to non-fissile isotopes will be presented. [4pt] [1] J. M. Mueller et al., Phys. Rev. C 85, 014605 (2012).

DETERMINATION OF REPORTABLE RADIONUCLIDES FOR DWPF SLUDGE BATCH 7B (MACROBATCH 9)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crawford, C. L.; Diprete, D. P.

The Waste Acceptance Product Specifications (WAPS) 1.2 require that “The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115”. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production throughmore » the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu- 242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 7a (SB7a) and Sludge Batch 7b (SB7b) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 9 (MB9). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the development of the Production Records that relate to radionuclide inventory. This work was initiated through Technical Task Request (TTR) HLW-DWPF-TTR-2011-0004; Rev. 0 entitled Sludge Batch 7b Qualification Studies. Specifically, this report details results from performing Subtask II, Item 2 of the TTR and, in part, meets Deliverable 6 of the TTR. The work was performed following the Task Technical and Quality Assurance Plan (TTQAP), SRNL-RP-2011-00247, Rev. 0 and Analytical Study Plan (ASP), SRNL-RP-2011-00248, Rev. 0. In order to determine the reportable radionuclides for SB7b (MB9), a list of radioisotopes that may meet the criteria as specified by the Department of Energy’s (DOE) WAPS was developed. All radioactive U- 235 fission products and all radioactive activation products that could be in the SRS HLW were considered. In addition, all U and Pu isotopes identified in WAPS 1.6 were included in the list. This list was then evaluated and some isotopes were excluded from the projection calculations. Based on measurements and analytical detection limits, 27 radionuclides have been identified as reportable for DWPF SB7b as specified by WAPS 1.2. The WCP and WQR require that all of the radionuclides present in the Design Basis glass be considered as the initial set of reportable radionuclides. For SB7b, all of the radionuclides in the Design Basis glass are reportable except for three radionuclides: Pd-107, Cs-135, and Th-230. At no time during the 1100- year period between 2015 and 3115 did any of these three radionuclides contribute to more than 0.01% of the radioactivity on a Curie basis. Two additional uranium isotopes (U-235 and -236) must be added to the list of reportable radionuclides in order to meet WAPS 1.6. All of the Pu isotopes (Pu-238, -239, -240, -241, and -242) and other U isotopes (U-233, -234, and -238) identified in WAPS 1.6 were already determined to be reportable according to WAPS 1.2 This brings the total number of reportable radionuclides for SB7b to 29. The radionuclide measurements made for SB7b are similar to those performed in the previous SB7a MB8 work. Some method development/refinement occurred during the conduct of these measurements, leading to lower detection limits and more accurate measurement of some isotopes than was previously possible. Improvement in the analytical measurements will likely continue, and this in turn should lead to improved detection limit values for some radionuclides and actual measurements for still others.« less

Determination Of Reportable Radionuclides For DWPF Sludge Batch 7B (Macrobatch 9)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Crawford, C. L.; DiPrete, D. P.

The Waste Acceptance Product Specifications (WAPS) 1.2 require that “The Producer shall report the inventory of radionuclides (in Curies) that have half-lives longer than 10 years and that are, or will be, present in concentrations greater than 0.05 percent of the total inventory for each waste type indexed to the years 2015 and 3115”. As part of the strategy to comply with WAPS 1.2, the Defense Waste Processing Facility (DWPF) will report for each waste type, all radionuclides (with half-lives greater than 10 years) that have concentrations greater than 0.01 percent of the total inventory from time of production throughmore » the 1100 year period from 2015 through 3115. The initial listing of radionuclides to be included is based on the design-basis glass as identified in the Waste Form Compliance Plan (WCP) and Waste Form Qualification Report (WQR). However, it is required that this list be expanded if other radionuclides with half-lives greater than 10 years are identified that may meet the greater than 0.01% criterion for Curie content. Specification 1.6 of the WAPS, International Atomic Energy Agency (IAEA) Safeguards Reporting for High Level Waste (HLW), requires that the ratio by weights of the following uranium and plutonium isotopes be reported: U-233, U-234, U-235, U-236, U-238, Pu-238, Pu-239, Pu-240, Pu-241, and Pu-242. Therefore, the complete set of reportable radionuclides must also include this set of U and Pu isotopes. The DWPF is receiving radioactive sludge slurry from HLW Tank 40. The radioactive sludge slurry in Tank 40 is a blend of the heel from Sludge Batch 7a (SB7a) and Sludge Batch 7b (SB7b) that was transferred to Tank 40 from Tank 51. The blend of sludge in Tank 40 is also referred to as Macrobatch 9 (MB9). This report develops the list of reportable radionuclides and associated activities as a function of time. The DWPF will use this list and the activities as one of the inputs for the development of the Production Records that relate to radionuclide inventory. This work was initiated through Technical Task Request (TTR) HLW-DWPF-TTR-2011-0004; Rev. 0 entitled Sludge Batch 7b Qualification Studies. Specifically, this report details results from performing Subtask II, Item 2 of the TTR and, in part, meets Deliverable 6 of the TTR. The work was performed following the Task Technical and Quality Assurance Plan (TTQAP), SRNL-RP-2011-00247, Rev. 0 and Analytical Study Plan (ASP), SRNL-RP-2011-00248, Rev. 0. In order to determine the reportable radionuclides for SB7b (MB9), a list of radioisotopes that may meet the criteria as specified by the Department of Energy’s (DOE) WAPS was developed. All radioactive U-235 fission products and all radioactive activation products that could be in the SRS HLW were considered. In addition, all U and Pu isotopes identified in WAPS 1.6 were included in the list. This list was then evaluated and some isotopes were excluded from the projection calculations. Based on measurements and analytical detection limits, 27 radionuclides have been identified as reportable for DWPF SB7b as specified by WAPS 1.2. The WCP and WQR require that all of the radionuclides present in the Design Basis glass be considered as the initial set of reportable radionuclides. For SB7b, all of the radionuclides in the Design Basis glass are reportable except for three radionuclides: Pd-107, Cs-135, and Th-230. At no time during the 1100-year period between 2015 and 3115 did any of these three radionuclides contribute to more than 0.01% of the radioactivity on a Curie basis. Two additional uranium isotopes (U-235 and -236) must be added to the list of reportable radionuclides in order to meet WAPS 1.6. All of the Pu isotopes (Pu-238, -239, -240, -241, and -242) and other U isotopes (U-233, -234, and -238) identified in WAPS 1.6 were already determined to be reportable according to WAPS 1.2 This brings the total number of reportable radionuclides for SB7b to 29. The radionuclide measurements made for SB7b are similar to those performed in the previous SB7a MB8 work. Some method development/refinement occurred during the conduct of these measurements, leading to lower detection limits and more accurate measurement of some isotopes than was previously possible. Improvement in the analytical measurements will likely continue, and this in turn should lead to improved detection limit values for some radionuclides and actual measurements for still others.« less

Photofission cross-section ratio measurement of 235 U/ 238 U using monoenergetic photons in the energy range of 9.0–16.6 MeV

DOE PAGES

Krishichayan,; Bhike, Megha; Finch, S. W.; ...

2017-05-01

Photofission cross-section ratios of 235U and 238U have been measured using monoenergetic photon beams from the High Intensity Gamma-ray Source facility at the Triangle Universities Nuclear Laboratory. These measurements have been performed in small energy steps between 9.0 and 16.6 MeV using a dual-fission ionization chamber. The measured cross-section ratios are compared with the previous experimental data as well as with the recent evaluated nuclear data library ENDF.

Production of neutron-rich nuclei approaching r-process by gamma-induced fission of 238U at ELI-NP

NASA Astrophysics Data System (ADS)

Mei, Bo; Balabanski, Dimiter; Constantin, Paul; Anh Le, Tuan; Viet Cuong, Phan

2018-05-01

The investigation of neutron-rich exotic nuclei is crucial not only for nuclear physics but also for nuclear astrophysics. Experimentally, only few neutron-rich nuclei near the stability have been studied, however, most neutron-rich nuclei have not been measured due to their small production cross sections as well as short half-lives. At ELI-NP, gamma beams with high intensities will open new opportunities to investigate very neutron-rich fragments produced by photofission of 238U targets in a gas cell. Based on some simulations, a novel gas cell has been designed to produce, stop and extract 238U photofission fragments. The extraction time and efficiency of photofission fragments have been optimized by using SIMION simulations. According to these simulations, a high extraction efficiency and a short extraction time can be achieved for 238U photofission fragments in the gas cell, which will allow one to measure very neutron-rich fragments with short half-lives by using the IGISOL facility proposed at ELI-NP.

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 MTE method is in the analytical performance achieved for the "minor" ratios 234U/238U and 236U/238U. The MTE method is now routinely used at all collaborating laboratories and possibly more in the future. Additional applications for the MTE method, e.g. to take advantage of the good external precision in combination with the possibilities of internal background and detector calibrations or mass jumps between different cup configurations, are presented as well. One interesting application concerns new absolute isotope ratio measurements for Ca with an unprecedented level of accuracy. This is important because up to now most reported Ca isotope data are only calculated as relative deviations from a standard like NIST-SRM 915. Using the MTE method measurements on new gravimetrically prepared Ca isotope mixtures were performed. A significantly improved level of accuracy at the level of about 0.02% for both the 42Ca/40Ca and 44Ca/40Ca ratios was obtained.

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

CONTROL SYSTEM FOR ISOTOPE SEPARATING APPARATUS

DOEpatents

Barnes, S.W.

1960-01-26

A method is described for controlling the position of the ion beams in a calutron used for isotope separation. The U/sup 238/ beams is centered over the U/sup 235/ receiving pocket, the operator monitoring the beam until a maximum reading is achieved on the meter connected to that pocket. Then both beams are simultaneously shifted by a preselected amount to move the U/sup 235/ beam over the U/sup 235/ pocket. A slotted door is placed over the entrance to that pocket during the U/sup 238/ beam centering to reduce the contamination to the pocket, while allowing enough beam to pass for monitoring purposes.

Fission Product Yields of 233U, 235U, 238U and 239Pu in Fields of Thermal Neutrons, Fission Neutrons and 14.7-MeV Neutrons

NASA Astrophysics Data System (ADS)

Laurec, J.; Adam, A.; de Bruyne, T.; Bauge, E.; Granier, T.; Aupiais, J.; Bersillon, O.; Le Petit, G.; Authier, N.; Casoli, P.

2010-12-01

The yields of more than fifteen fission products have been carefully measured using radiochemical techniques, for 235U(n,f), 239Pu(n,f) in a thermal spectrum, for 233U(n,f), 235U(n,f), and 239Pu(n,f) reactions in a fission neutron spectrum, and for 233U(n,f), 235U(n,f), 238U(n,f), and 239Pu(n,f) for 14.7 MeV monoenergetic neutrons. Irradiations were performed at the EL3 reactor, at the Caliban and Prospero critical assemblies, and at the Lancelot electrostatic accelerator in CEA-Valduc. Fissions were counted in thin deposits using fission ionization chambers. The number of fission products of each species were measured by gamma spectrometry of co-located thick deposits.

In-beam Fission Study at JAEA

NASA Astrophysics Data System (ADS)

Nishio, Katsuhisa

2013-12-01

Fission fragment mass distributions were measured in heavy-ion induced fissions using 238U target nucleus. The measured mass distributions changed drastically with incident energy. The results are explained by a change of the ratio between fusion and quasifission with nuclear orientation. A calculation based on a fluctuation dissipation model reproduced the mass distributions and their incident energy dependence. Fusion probability was determined in the analysis. Evaporation residue cross sections were calculated with a statistical model in the reactions of 30Si + 238U and 34S + 238U using the obtained fusion probability in the entrance channel. The results agree with the measured cross sections for seaborgium and hassium isotopes.

In-beam fission study for Heavy Element Synthesis

NASA Astrophysics Data System (ADS)

Nishio, Katsuhisa

2013-12-01

Fission fragment mass distributions were measured in heavy-ion induced fissions using 238U target nucleus. The measured mass distributions changed drastically with incident energy. The results are explained by a change of the ratio between fusion and qasifission with nuclear orientation. A calculation based on a fluctuation dissipation model reproduced the mass distributions and their incident energy dependence. Fusion probability was determined in the analysis. Evaporation residue cross sections were calculated with a statistical model in the reactions of 30Si + 238U and 34S + 238U using the obtained fusion probability in the entrance channel. The results agree with the measured cross sections for seaborgium and hassium isotopes.

Evaluating steady-state soil thickness by coupling uranium series and 10Be cosmogenic radionuclides

NASA Astrophysics Data System (ADS)

Vanacker, Veerle; Schoonejans, Jerome; Opfergelt, Sophie; Granet, Matthieu; Christl, Marcus; Chabaux, Francois

2017-04-01

Within the Critical Zone, the development of the regolith mantle is controlled by the downwards propagation of the weathering front into the bedrock and denudation at the surface of the regolith by mass movements, water and wind erosion. When the removal of surface material is approximately balanced by the soil production, the soil system is assumed to be in steady-state. The steady state soil thickness (or so-called SSST) can be considered as a dynamic equilibrium of the system, where the thickness of the soil mantle stays relatively constant over time. In this study, we present and compare analytical data from two independent isotopic techniques: in-situ produced cosmogenic nuclides and U-series disequilibria to constrain soil development under semi-arid climatic conditions. The Spanish Betic Cordillera (Southeast Spain) was selected for this study, as it offers us a unique opportunity to analyze soil thickness steady-state conditions for thin soils of semiarid environments. Three soil profiles were sampled across the Betic Ranges, at the ridge crest of zero-order catchments with distinct topographic relief, hillslope gradient and 10Be-derived denudation rate. The magnitude of soil production rates determined based on U-series isotopes (238U, 234U, 230Th and 226Ra) is in the same order of magnitude as the 10Be-derived denudation rates, suggesting steady state soil thickness in two out of three sampling sites. The results suggest that coupling U-series isotopes with in-situ produced radionuclides can provide new insights in the rates of soil development; and also illustrate the potential frontiers in applying U-series disequilibria to track soil production in rapidly eroding landscapes characterized by thin weathering depths.

Mass-yield distributions of fission products from 20, 32, and 45 MeV proton-induced fission of 232Th

NASA Astrophysics Data System (ADS)

Naik, H.; Goswami, A.; Kim, G. N.; Kim, K.; Suryanarayana, S. V.

2013-10-01

The yields of various fission products in the 19.6, 32.2, and 44.8 MeV proton-induced fission of 232Th have been determined by recoil catcher and an off-line γ-ray spectrometric technique using the BARC-TIFR Pelletron in India and MC-50 cyclotron in Korea. The mass-yield distributions were obtained from the fission product yield using the charge distribution corrections. The peak-to-valley (P/V) ratio of the present work and that of literature data for 232Th(p,f) and 238U(p,f) were obtained from the mass yield distribution. The present and the existing literature data for 232Th(p,f), 232Th(n,f), and 232Th( γ,f) at various energies were compared with those for 238U(p,f), 238U(n,f), and 238U( γ,f) to examine the probable nuclear structure effect. The role of Th-anomaly on the peak-to-valley ratio in proton-, neutron-, and photon-induced fission of 232Th was discussed with the similar data in 238U. On the other hand, the fine structure in the mass yield distributions of the fissioning systems at various excitation energies has been explained from the point of standard I and II asymmetric mode of fission besides the probable role of even-odd effect, A/ Z ratio, and fissility parameter.

Ages of subsurface stratigraphic intervals in the Quaternary of Enewetak Atoll, Marshall Islands

USGS Publications Warehouse

Szabo, B. J.; Tracey, J.I.; Goter, E.R.

1985-01-01

Drill cores of Enewetak Atoll, Marshall Islands, reveal six stratigraphic intervals, numbered in downward sequence, which represent vertical coral growth during Quaternary interglaciations. Radiocarbon dates indicate that the Holocene sea transgressed the emergent reef platform by about 8000 yr B.P. The reef grew rapidly upward (about 5 to 10 mm/yr) until about 6500 yr B.P. Afterward vertical growth slowed to about 0.5 mm/yr, then lateral development became dominant during the last several thousand years. The second interval is dated at 131,000 ?? 3000 yr B.P. by uranium series. This unit correlates with oxygen-isotope substage 5e and with terrace VIIa of Huon Peninsula, New Guinea, and of Main Reef-2 terrace at Atauro Island. The third interval is not dated because corals were recrystallized and it is tentatively correlated with either oxygen-isotope stages 7 or 9. The age of the fourth interval is estimated at 454,000 ?? 100,000 yr B.P. from measured 234U 238U activity ratios. This unit is correlated with either oxygen-isotope stage 9, 11, or 13. ?? 1985.

Preparation of alpha sources using magnetohydrodynamic electrodeposition for radionuclide metrology.

PubMed

Panta, Yogendra M; Farmer, Dennis E; Johnson, Paula; Cheney, Marcos A; Qian, Shizhi

2010-02-01

Expanded use of nuclear fuel as an energy resource and terrorist threats to public safety clearly require the development of new state-of-the-art technologies and improvement of safety measures to minimize the exposure of people to radiation and the accidental release of radiation into the environment. The precision in radionuclide metrology is currently limited by the source quality rather than the detector performance. Electrodeposition is a commonly used technique to prepare massless radioactive sources. Unfortunately, the radioactive sources prepared by the conventional electrodeposition method produce poor resolution in alpha spectrometric measurements. Preparing radioactive sources with better resolution and higher yield in the alpha spectrometric range by integrating magnetohydrodynamic convection with the conventional electrodeposition technique was proposed and tested by preparing mixed alpha sources containing uranium isotopes ((238)U, (234)U), plutonium ((239)Pu), and americium ((241)Am) for alpha spectrometric determination. The effects of various parameters such as magnetic flux density, deposition current and time, and pH of the sample solution on the formed massless radioactive sources were also experimentally investigated. Copyright 2009 Elsevier Inc. All rights reserved.

Study of a generalized birks formula for the scintillation response of a CaMoO4 crystal

NASA Astrophysics Data System (ADS)

Lee, J. Y.; Kim, H. J.; Kang, Sang Jun; Lee, M. H.

2017-12-01

We have investigated the scintillation characteristics of CaMoO4 (CMO) crystals by using a gamma source and various internal alpha sources. A 137Cs source with 662-keV gamma-rays was used for the gamma-quanta light yield calibration. Internal radioactive contaminations provided alpha particles with different energies from 5.41 to 7.88 MeV. We developed a C++ program based on the ROOT package for the fitting of parameters in a generalized Birks semi-empirical formula by combining the experimental and the simulation data. Results for the fitted Birks parameters are k b1 = 3.3 × 10 -3 (g/MeVcm2) for the 1st parameter and k b2 = 7.9 × 10 -5 (g/MeVcm2)2 for the 2nd parameter. The χ2/n.d.f. (Number of Degree of Freedom) is calculated as 0.1/4. We were able to estimate the 238U and 234U contaminations in a CMO crystal by using the generalized Birks semi-empirical formula.

U-238-U-234-Th-230-Th-232 systematics and the precise measurement of time over the past 500,000 years

NASA Technical Reports Server (NTRS)

Edwards, R. Lawrence; Chen, J. H.; Wasserburg, G. J.

1987-01-01

A method is presented for the high-precision measurement of the Th-230 abundance in corals by isotope-dilution mass spectrometry using techniques developed by Chen and Wasserburg (1980, 1981) and Chen et al. (1986). It is shown that 6 x 10 to the 8th atoms of Th-230 can be measured to + or - 30 percent (2 sigma) and 2 x 10 to the 10th atoms of Th-230 to + or - 2 percent. The time over which useful age data on corals can be obtained ranges from a few years to about 500 ky, with the uncertainty in age ranging from 5 y for a 180-y-old coral, to 44 y for a 8294-y-old coral, to 1.1 ky for a 123.1-ky-old coral. Ages were determined with high analytical precision for several corals that grew during high sea-level stands about 120 ky ago, supporting the view that the dominant cause of Pleistocene climate change was Milankovitch forcing.

Depth profile of 236U/238U in soil samples in La Palma, Canary Islands

PubMed Central

Srncik, M.; Steier, P.; Wallner, G.

2011-01-01

The vertical distribution of the 236U/238U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the 240Pu/239Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios 236U/238U, 240Pu/239Pu and 236U/239Pu, respectively. The 236U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio 240Pu/239Pu indicated a global fallout signature we assume the same origin as the probable source for 236U. Our measured 236U/239Pu value of around 0.2 is within the expected range for this contamination source. PMID:21481502

U-Pb ages of secondary silica at Yucca Mountain, Nevada: Implications for the paleohydrology of the unsaturated zone

USGS Publications Warehouse

Neymark, L.A.; Amelin, Y.; Paces, J.B.; Peterman, Z.E.

2002-01-01

Uranium, Th and Pb isotopes were analyzed in layers of opal and chalcedony from individual mm- to cm-thick calcite and silica coatings at Yucca Mountain, Nevada, USA, a site that is being evaluated for a potential high-level nuclear waste repository. These calcite and silica coatings on fractures and in lithophysal cavities in Miocene-age tuffs in the unsaturated zone (UZ) precipitated from descending water and record a long history of percolation through the UZ. Opal and chalcedony have high concentrations of U (10 to 780 ppm) and low concentrations of common Pb as indicated by large values of 206Pb/204Pb (up to 53,806), thus making them suitable for U-Pb age determinations. Interpretations of U-Pb isotope systems in opal samples at Yucca Mountain are complicated by the incorporation of excess 234U at the time of mineral formation, resulting in reverse discordance of U-Pb ages. However, the 207PB/235U ages are much less affected by deviation from initial secular equilibrium and provide reliable ages of most silica deposits between 0.6 and 9.8 Ma. For chalcedony subsamples showing normal age discordance, these ages may represent minimum times of deposition. Typically, 207Pb/235U ages are consistent with the microstratigraphy in the mineral coating samples, such that the youngest ages are for subsamples from outer layers, intermediate ages are from inner layers, and oldest ages are from innermost layers. 234U and 230Th in most silica layers deeper in the coatings are in secular equilibrium with 238U, which is consistent with their old age and closed system behavior during the past -0.5 Ma. The ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from lithophysal cavities in the welded part of the Topopah Spring Tuff yield slow long-term average growth rates of 1 to 5 mm/Ma. These data imply that the deeper parts of the UZ at Yucca Mountain maintained long-term hydrologic stability over the past 10 Ma. despite significant climate variations. U-Pb ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from fractures in the shallower part of the UZ (welded part of the overlying Tiva Canyon Tuff) indicate larger long-term average growth rates up to 23 mm/Ma and an absence of recently deposited materials (ages of outermost layers are 3-5 Ma.). These differences between the characteristics of the coatings for samples from the shallower and deeper parts of the UZ may indicate that the nonwelded tuffs (PTn), located between the welded parts of the Tiva Canyon and Topopah Spring Tuffs, play an important role in moderating UZ flow.

Prototype development of ion exchanging alpha detectors

NASA Astrophysics Data System (ADS)

Krupp, Dominik; Scherer, Ulrich W.

2018-07-01

In contemporary alpha particle spectrometry, the sample preparation is separated from the detection of the radionuclides. The sample preparation itself requires much time and the equipment of a radiochemistry lab. If sample preparation and detection could be combined in one step, a huge time-saving potential becomes available. One way to realize such a combination is described here. The concept was explored by simulations with the well-established computer programs SRIM and AASI. In a proof of concept, the active surface of commercially available alpha detectors was modified with sulfonic acid groups as a well-known type of cation exchanger. It was shown, that in contrast to a pristine detector, a chemically modified detector is able to extract uranium-238 and -234 selectively as uranyl cations onto the detector surface from a diluted [238/234U]uranyl acetate solution. It was possible to measure directly in the sample solution for one week or to prepare the modified detector surfaces within 30 s for measurements in conventional alpha chambers. In either case, the full width at half maximum of the measured spectra was around 100 keV, allowing a clear nuclide identification. After regenerating the cation exchanger surfaces by rinsing with hydrochloric acid the typical uranium spectra had disappeared, proving chemical bonding of the uranium. Due to the large variety of potential functional groups this new way of alpha spectrometry could be beneficial for all fields of alpha particle spectrometry, from environmental analysis, over security measurements to studies of the heaviest elements.

Accurate 238U(n , 2 n )237U reaction cross-section measurements from 6.5 to 14.8 MeV

NASA Astrophysics Data System (ADS)

Krishichayan, Bhike, M.; Tornow, W.; Tonchev, A. P.; Kawano, T.

2017-10-01

The cross section for the 238U(n ,2 n )237U reaction has been measured in the incident neutron energy range from 6.5 to 14.8 MeV in small energy steps using an activation technique. Monoenergetic neutron beams were produced via the 2H(d ,n )3He and 3H(d ,n )4He reactions. 238U targets were activated along with Au and Al monitor foils to determine the incident neutron flux. The activity of the reaction products was measured in TUNL's low-background counting facility using high-resolution γ -ray spectroscopy. The results are compared with previous measurements and latest data evaluations. Statistical-model calculations, based on the Hauser-Feshbach formalism, have been carried out using the CoH3 code and are compared with the experimental results. The present self-consistent and high-quality data are important for stockpile stewardship and nuclear forensic purposes as well as for the design and operation of fast reactors.

Validation of uranium determination in urine by ICP-MS.

PubMed

Bouvier-Capely, C; Baglan, N; Montègue, A; Ritt, J; Cossonnet, C

2003-08-01

A rapid procedure--dilution of urine+ICP-MS measurement--for the determination of uranium in urine was validated. Large ranges of concentration and isotopic composition were studied on urine samples excreted by occupationally exposed workers. The results were consistent with those obtained by fluorimetry and by alpha spectrometry after a purification procedure, two currently used techniques. However, the proposed procedure is limited for determination of the minor isotope 234U. Thus for worker monitoring, the conversion of 234U mass concentration into activity concentration can lead to an erroneous value of the effective dose, in particular for a contamination at very low level with highly enriched uranium. A solution to avoid this hazard is to perform a chemical purification prior to ICP-MS measurement to lower uncertainty and detection limit for 234U.

Reexamining the heavy-ion reactions 238U+238U and 238U+248Cm and actinide production close to the barrier

NASA Astrophysics Data System (ADS)

Kratz, J. V.; Schädel, M.; Gäggeler, H. W.

2013-11-01

Recent theoretical work has renewed interest in radiochemically determined isotope distributions in reactions of 238U projectiles with heavy targets that had previously been published only in parts. These data are being reexamined. The cross sections σ(Z) below the uranium target have been determined as a function of incident energy in thick-target bombardments. These are compared to predictions by a diffusion model whereby consistency with the experimental data is found in the energy intervals 7.65-8.30 MeV/u and 6.06-7.50 MeV/u. In the energy interval 6.06-6.49 MeV/u, the experimental data are lower by a factor of 5 compared to the diffusion model prediction indicating a threshold behavior for massive charge and mass transfer close to the barrier. For the intermediate energy interval, the missing mass between the primary fragment masses deduced from the generalized Qgg systematics including neutron pair-breaking corrections and the centroid of the experimental isotope distributions as a function of Z have been used to determine the average excitation energy as a function of Z. From this, the Z dependence of the average total kinetic-energy loss (TKEL¯) has been determined. This is compared to that measured in a thin-target counter experiment at 7.42 MeV/u. For small charge transfers, the values of TKEL¯ of this work are typically about 30 MeV lower than in the thin-target experiment. This difference is decreasing with increasing charge transfer developing into even slightly larger values in the thick-target experiment for the largest charge transfers. This is the expected behavior which is also found in a comparison of the partial cross sections for quasielastic and deep-inelastic reactions in both experiments. The cross sections for surviving heavy actinides, e.g., 98Cf, 99Es, and 100Fm indicate that these are produced in the low-energy tails of the dissipated energy distributions, however, with a low-energy cutoff at about 35 MeV. Excitation functions show that identical isotope distributions are populated independent of the bombarding energy indicating that the same bins of excitation energy are responsible for the production of these fissile isotopes. A comparison of the survival probabilities of the residues of equal charge and neutron transfers in the reactions of 238U projectiles with either 238U or 248Cm targets is consistent with such a cutoff as evaporation calculations assign the surviving heavy actinides to the 3n and/or 4n evaporation channels.

Rapid Method for Sodium Hydroxide Fusion of Concrete and ...

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

Relativistic Coulomb Fission

NASA Technical Reports Server (NTRS)

Norbury, John W.

1992-01-01

Nuclear fission reactions induced by the electromagnetic field of relativistic nuclei are studied for energies relevant to present and future relativistic heavy ion accelerators. Cross sections are calculated for U-238 and Pu-239 fission induced by C-12, Si-28, Au-197, and U-238 projectiles. It is found that some of the cross sections can exceed 10 b.

Assay Methods for 238U, 232Th, and 210Pb in Lead and Calibration of 210Bi Bremsstrahlung Emission from Lead

DOE Office of Scientific and Technical Information (OSTI.GOV)

Orrell, John L.; Aalseth, Craig E.; Arnquist, Isaac J.

2016-02-13

Assay methods for measuring 238U, 232Th, and 210Pb concentrations in refined lead are presented. The 238U and 232Th concentrations are assayed via inductively coupled plasma mass spectrometry (ICP-MS) after anion exchange column separation on dissolved lead samples. The 210Pb concentration is inferred through α-spectroscopy of a daughter isotope, 210Po, after chemical precipitation separation on dissolved lead samples. Subsequent to the 210Po α-spectroscopy assay, a method for evaluating 210Pb concentrations in solid lead samples was developed via measurement of bremsstrahlung radiation from β-decay of a daughter isotope, 210Bi, by employing a 14-crystal array of high purity germanium (HPGe) detectors. Ten sourcesmore » of refined lead were assayed. The 238U concentrations were <34 microBq/kg and the 232Th concentrations ranged <0.6 – 15 microBq/kg, as determined by the ICP-MS assay method. The 210Pb concentrations ranged from ~0.1 – 75 Bq/kg, as inferred by the 210Po α-spectroscopy assay method.« less

EXAFS Reveals the Mechanism of U Isotope Fractionation During Adsorption to Mn Oxyhydroxide

NASA Astrophysics Data System (ADS)

Wasylenki, L. E.; Brennecka, G.; Bargar, J.; Weyer, S.; Anbar, A. D.

2010-12-01

Natural variations in the ratio of 238U/235U due to “stable” isotope fractionation have now been reported for a range of geological samples [1-3]. Among the observed variations are a small difference in 238U/235U between seawater and ferromanganese sediments (seawater slightly heavier) and a larger difference, with opposite sense, between seawater and black shales (seawater lighter). These variations suggest that long-term changes in the proportions of oxic and anoxic/sulfidic sinks for U in the ocean over Earth’s history may be recorded as shifts in the isotopic compositions of marine sediments. Thus U isotopes are a potential paleoredox proxy for the oceans, as suggested by [4]. In order to investigate the mechanism behind fractionation of U isotopes in oxidizing marine environments, we previously conducted simple adsorption experiments in which an isotopically known pool of dissolved U partly adsorbed onto synthetic birnessite, a common Mn oxyhydroxide in hydrogenetic ferromanganese crusts. Our experimental result agreed very well with that observed between seawater and natural ferromanganese sediments: δ238U/235U of adsorbed U was 0.2‰ lighter than δ238U/235U of dissolved U [5]. The magnitude of fractionation is constant as a function of experimental duration and fraction of U adsorbed, suggesting an equilibrium isotope effect. Many metal isotope effects are driven by changes in oxidation state for the metal of interest. Because both dissolved and adsorbed U are hexavalent in this system, a redox reaction cannot be causing isotope fractionation. We therefore hypothesized that a difference in uranium’s coordination environment between dissolved and adsorbed U is likely responsible for the isotope effect. We analyzed a sample from our experimental study with extended X-ray absorption fine structure (EXAFS) spectroscopy. Comparison of the EXAFS spectrum of U adsorbed on birnessite with the spectra of aqueous U species (UO22+ and UO2(CO3)34-) reveals subtle, but important differences in the U-O coordination shell between dissolved and adsorbed U. In particular, there is an increase in disorder in the bond distances to equatorial oxygens in the adsorbed complex. Our EXAFS data support our hypothesis that a difference in coordination chemistry drives the isotope effect observed in our experiments. The same mechanism may well explain the U isotope fractionation observed between seawater and hydrogenetic ferromanganese nodules, although a similar investigation of U isotope behavior during adsorption to Fe oxyhydroxides should be undertaken. [1] Weyer et al. (2008) GCA 72, 345. [2] Stirling et al. (2007) EPSL 264, 208. [3] Bopp et al. (2009) Geology, 37, 611. [4] Montoya-Pino et al. (2010) Geology 38, 315. [5] Brennecka et al. (2008) GCA 72(12) Suppl., A114.

Field analyses of (238)U and (226)Ra in two uranium mill tailings piles from Niger using portable HPGe detector.

PubMed

Déjeant, Adrien; Bourva, Ludovic; Sia, Radia; Galoisy, Laurence; Calas, Georges; Phrommavanh, Vannapha; Descostes, Michael

2014-11-01

The radioactivities of (238)U and (226)Ra in mill tailings from the U mines of COMINAK and SOMAÏR in Niger were measured and quantified using a portable High-Purity Germanium (HPGe) detector. The (238)U and (226)Ra activities were measured under field conditions on drilling cores with 600s measurements and without any sample preparation. Field results were compared with those obtained by Inductive Coupled Plasma Atomic Emission Spectroscopy (ICP-AES) and emanometry techniques. This comparison indicates that gamma-ray absorption by such geological samples does not cause significant deviations. This work shows the feasibility of using portable HPGe detector in the field as a preliminary method to observe variations of radionuclides concentration with the aim of identifying samples of interest. The HPGe is particularly useful for samples with strong secular disequilibrium such as mill tailings. Copyright © 2014 Elsevier Ltd. All rights reserved.

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 isotope ratios. These results suggest that the rate-limited transport properties of U in the Rifle aquifer are governed by the presence of low-permeability regions in the modeling domain and that these zones are responsible for the suggested "memory" effect observed in previous U isotope studies at this site.

First Conclusions of the WPEC/Subgroup-22 Nuclear Data for Improved LEU-LWR Reactivity Predictions

NASA Astrophysics Data System (ADS)

Courcelle, Arnaud

2005-05-01

This paper is a summary of a collective work in the framework of the Working Party in International Nuclear Data Evaluation and Co-operation (WPEC) to investigate the reasons for systematic reactivity underprediction of thermal LEU-LWR (Low-Enriched Uranium, Light-Water Reactor). This keff underprediction (≈ -500 pcm) is observed with the most recent nuclear data libraries (ENDF/B-VI.8, JENDL3.3 and JEFF3.0) This report reviews the evaluation work performed at several laboratories [Oak Ridge National Laboratory (ORNL), Los Alamos National Laboratory (LANL), Commissariat a l'énergie atomique de Bruyeres-Le-Chatel (CEA-BRC), International Atomic Energy Agency (IAEA)] as well as the integral tests (mainly at LANL, Knoll Atomic Power Laboratory (KAPL), Bettis Atomic Power Laboratory (BAPL), Nuclear Research and Consultancy Group NRG-Petten, CEA and IAEA) of the successive versions of the new evaluated files. The present status of the work can be summarized as follows: • Improved evaluations of 238U inelastic data proposed by LANL and CEA-BRC were tested against integral benchmarks and partially improve the reactivity prediction. • The thermal capture cross-section of 238U has been revised, and a new evaluation of 238U resonance parameters, up to 20 keV, is in progress at ORNL. Integral tests have ensured that the modifications of 238U capture cross-section in the thermal and resolved range were still compatible with 238U integral measurements (238U capture rate ratios measured in critical facilities and 239Pu build-up prediction in a depleted pressurized water reactor (PWR) assembly). It is demonstrated that the combination of the new inelastic data (LANL or BRC) with the preliminary ORNL resonance parameter set gives a good correction of the reactivity under-estimation. The provisional conclusions of this collective work are expected to contribute toward the improvement of the future versions of nuclear data libraries.

Reactive transport of uranium in a groundwater bioreduction study: Insights from high-temporal resolution 238U/235U data

NASA Astrophysics Data System (ADS)

Shiel, A. E.; Johnson, T. M.; Lundstrom, C. C.; Laubach, P. G.; Long, P. E.; Williams, K. H.

2016-08-01

We conducted a detailed investigation of U isotopes in conjunction with a broad geochemical investigation during field-scale biostimulation and desorption experiments. This investigation was carried out in the uranium-contaminated alluvial aquifer of the Rifle field research site. In this well-characterized setting, a more comprehensive understanding of U isotope geochemistry is possible. Our results indicate that U isotope fractionation is consistently observed across multiple experiments at the Rifle site. Microbially-mediated reduction is suggested to account for most or all of the observed fractionation as abiotic reduction has been demonstrated to impart much smaller, often near-zero, isotopic fractionation or isotopic fractionation in the opposite direction. Data from some time intervals are consistent with a simple model for transport and U(VI) reduction, where the fractionation factor (ε = +0.65‰ to +0.85‰) is consistent with experimental studies. However, during other time intervals the observed patterns in our data indicate the importance of other processes in governing U concentrations and 238U/235U ratios. For instance, we demonstrate that departures from Rayleigh behavior in groundwater systems arise from the presence of adsorbed species. We also show that isotope data are sensitive to the onset of oxidation after biostimulation ends, even in the case where reduction continues to remove contaminant uranium downstream. Our study and the described conceptual model support the use of 238U/235U ratios as a tool for evaluating the efficacy of biostimulation and potentially other remedial strategies employed at Rifle and other uranium-contaminated sites.

Study of 236U/238U ratio at CIRCE using a 16-strip silicon detector with a TOF system

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Gialanella, L.; Terrasi, F.

2015-04-01

Accelerator Mass Spectrometry (AMS) is presently the most sensitive technique for the measurement of long-lived actinides, e.g. 236U and xPu isotopes. A new actinide AMS system, based on a 3-MV pelletron tandem accelerator, is operated at the Center for Isotopic Research on Cultural and Environmental Heritage (CIRCE) in Caserta, Italy. In this paper we report on the procedure adopted to increase the 236U abundance sensitivity as low as possible. The energy and position determinations of the 236U ions, using a 16-strip silicon detector have been obtained. A 236U/238U isotopic ratio background level of about 2.9×10-11 was obtained, summing over all the strips, using a Time of Flight-Energy (TOF-E) system with a 16-strip silicon detector (4.9×10-12 just with one strip).

Geochemical gradients within modern and fossil shells of Concholepas concholepas from northern Chile: an insight into U-Th systematics and diagenetic/authigenic isotopic imprints in mollusk shells

NASA Astrophysics Data System (ADS)

Labonne, Maylis; Hillaire-Marcel, Claude

2000-05-01

Seriate geochemical measurements through shells of one modern, one Holocene, and two Sangamonian Concholepas concholepas, from marine terraces of Northern Chile, were performed to document diagenetic vs. authigenic geochemical signatures, and to better interpret U-series ages on such material. Subsamples were recovered by drilling from the outer calcitic layer to the inner aragonitic layer of each of the studied shells. Unfortunately, this sampling procedure induces artifacts, notably the convertion of up to ˜20% of calcite into aragonite, and of up to ˜6% of aragonite into calcite, as well as in the epimerization of a few percent of isoleucine into D-alloisoleucine/ L-isoleucine. Negligible sampling artifacts were noticed for stable isotope and total amino acid contents. Diagenetic effects on the geochemical properties of the shells are particularly pronounced in the inner aragonitic layer and more discrete in the outer calcitic layer. The time-dependent decay of the organic matrix of the shell is illustrated by a one order of magnitude lower total amino acid content in the Sangamonian specimens by comparison with the modern shell. Conversely, the Sangamonian shells U contents increase by a similar factor and 13C- 18O enrichments as high as 2 to 3‰ seem also to occur through the same time interval possibly due to partial replacement of aragonite by gypsum. The decay of the organic matrix of the aragonitic layer of the shell is thought to play a major role with respect to U-uptake processes and stable isotope shifts. Nevertheless, asymptotic 230Th-ages (˜100 ka) in the inner U-rich layers of the Sangamonian shells, and 234U/ 238U ratios compatible with a marine origin for U, suggest U-uptake within a short diagenetic interval, when marine waters were still bathing the embedding sediment. Thus, U-series ages on fossil mollusks from such a hyper-arid environment should not differ much from the age of the corresponding marine unit deposition. However, the diagenetic enrichments in stable isotopes raise concerns about their use for paleoenvironmental reconstructions under such climate conditions.

Measurements of charge state distributions of 0.74 and 1.4 MeV /u heavy ions passing through dilute gases

NASA Astrophysics Data System (ADS)

Scharrer, P.; Düllmann, Ch. E.; Barth, W.; Khuyagbaatar, J.; Yakushev, A.; Bevcic, M.; Gerhard, P.; Groening, L.; Horn, K. P.; Jäger, E.; Krier, J.; Vormann, H.

2017-04-01

In many modern heavy-ion accelerator facilities, gas strippers are used to increase the projectile charge state for improving the acceleration efficiency of ion beams to higher energies. For this application, the knowledge on the behavior of charge state distributions of heavy-ions after passing through dilute gases is of special interest. Charge state distributions of uranium (238U), bismuth (209Bi), titanium (50Ti), and argon (40Ar) ion beams with energies of 0.74 MeV /u and 1.4 MeV /u after passing through hydrogen (H2 ), helium (He), carbon dioxide (CO2 ), nitrogen (N2 ), oxygen (O2 ), neon (Ne), and argon (Ar) gases were measured. Gas stripper target thicknesses up to 100 μ g /cm2 were applied. The observed behavior of the charge state distributions, including their width and mean charge state, are discussed. The measurements show the highest equilibrium charge state at 1.4 MeV /u for 238U on H2 gas of 29.2 ±1.2 . Narrow charge state distributions are observed for 238U and 209Bi on H2 and He gas, which are highly beneficial, e.g., for the production of beams of high intensities in accelerators.

Analysis of benchmark critical experiments with ENDF/B-VI data sets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hardy, J. Jr.; Kahler, A.C.

1991-12-31

Several clean critical experiments were analyzed with ENDF/B-VI data to assess the adequacy of the data for U{sup 235}, U{sup 238} and oxygen. These experiments were (1) a set of homogeneous U{sup 235}-H{sub 2}O assemblies spanning a wide range of hydrogen/uranium ratio, and (2) TRX-1, a simple, H{sub 2}O-moderated Bettis lattice of slightly-enriched uranium metal rods. The analyses used the Monte Carlo program RCP01, with explicit three-dimensional geometry and detailed representation of cross sections. For the homogeneous criticals, calculated k{sub crit} values for large, thermal assemblies show good agreement with experiment. This supports the evaluated thermal criticality parameters for U{supmore » 235}. However, for assemblies with smaller H/U ratios, k{sub crit} values increase significantly with increasing leakage and flux-spectrum hardness. These trends suggest that leakage is underpredicted and that the resonance eta of the ENDF/B-VI U{sup 235} is too large. For TRX-1, reasonably good agreement is found with measured lattice parameters (reaction-rate ratios). Of primary interest is rho28, the ratio of above-thermal to thermal U{sup 238} capture. Calculated rho28 is 2.3 ({+-} 1.7) % above measurement, suggesting that U{sup 238} resonance capture remains slightly overpredicted with ENDF/B-VI. However, agreement is better than observed with earlier versions of ENDF/B.« less

Photon-induced Fission Product Yield Measurements on 235U, 238U, and 239Pu

NASA Astrophysics Data System (ADS)

Krishichayan, Fnu; Bhike, M.; Tonchev, A. P.; Tornow, W.

2015-10-01

During the past three years, a TUNL-LANL-LLNL collaboration has provided data on the fission product yields (FPYs) from quasi-monoenergetic neutron-induced fission of 235U, 238U, and 239Pu at TUNL in the 0.5 to 15 MeV energy range. Recently, we have extended these experiments to photo-fission. We measured the yields of fission fragments ranging from 85Kr to 147Nd from the photo-fission of 235U, 238U, and 239Pu using 13-MeV mono-energetic photon beams at the HIGS facility at TUNL. First of its kind, this measurement will provide a unique platform to explore the effect of the incoming probe on the FPYs, i.e., photons vs. neutrons. A dual-fission ionization chamber was used to determine the number of fissions in the targets and these samples (along with Au monitor foils) were gamma-ray counted in the low-background counting facility at TUNL. Details of the experimental set-up and results will be presented and compared to the FPYs obtained from neutron-induced fission at the same excitation energy of the compound nucleus. Work supported in part by the NNSA-SSAA Grant No. DE-NA0001838.

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.

U-Pb ages of uraniferous opals and implications for the history of beryllium, fluorine, and uranium mineralization at Spor Mountain, Utah

USGS Publications Warehouse

Ludwig, K. R.; Lindsey, D.A.; Zielinski, R.A.; Simmons, K.R.

1980-01-01

The U-Pb isotope systematics of uraniferous opals from Spor Mountain, Utah, were investigated to determine the suitability of such material for geochronologic purposes, and to estimate the timing of uranium and associated beryllium and fluorine mineralization. The results indicate that uraniferous opals can approximate a closed system for uranium and uranium daughters, so that dating samples as young as ???1 m.y. should be possible. In addition, the expected lack of initial 230Th and 231Pa in opals permits valuable information on the initial 234U/238U to be obtained on suitable samples of ???10 m.y. age. The oldest 207Pb/235U apparent age observed, 20.8 ?? 1 m.y., was that of the opal-fluorite core of a nodule from a beryllium deposit in the Spor Mountain Formation. This age is indistinguishable from that of fission-track and K-Ar ages from the host rhyolite, and links the mineralization to the first episode of alkali rhyolite magmatism and related hydrothermal activity at Spor Mountain. Successively younger ages of 13 m.y. and 8-9 m.y. on concentric outer zones of the same nodule indicate that opal formed either episodically or continuously for over 10 m.y. Several samples of both fracture-filling and massive-nodule opal associated with beryllium deposits gave 207Pb/235U apparent ages of 13-16 m.y., which may reflect a restricted period of mineralization or perhaps an averaging of 21- and <13-m.y. periods of opal growth. Several samples of fracture-filling opal in volcanic rocks as young as 6 m.y. gave 207Pb/235U ages of 3.4-4.8 m.y. These ages may reflect hot-spring activity after the last major eruption of alkali rhyolite. ?? 1980.

Upwelling Rates Beneath Hotspots : Evidence From U-Series in Basalts From the Mid-Atlantic Ridge and the Azores Islands

NASA Astrophysics Data System (ADS)

Bourdon, B. P.; Turner, S. P.

2001-12-01

In this study, we have analyzed U-series in lavas from the Azores islands and the nearby Mid-Atlantic Ridge (FAZAR cruise) in an attempt to assess the relative importance of melting processes versus source variations in the context of ridge-hotpsot interaction. The lavas were analyzed for 238U-230Th (Turner et al. 1997, Bourdon et al. 1996) 226Ra-230Th and 235U-231Pa disequilibria by thermal ionisation mass spectrometry. Our results for the historic lavas from the Azores islands show that the 231Pa excess are at the low end of the trend found for other OIB (Pickett et al. 1997 and Bourdon et al. 1998) and fall on a positive correlation in a 231Pa/235U versus 230Th/238U diagram. In contrast, lavas from the nearby Mid-Atlantic ridge are characterized by larger (231Pa/235U) activity ratios for similar and greater (230Th/238U) ratios. There is also a weak correlation between 226Ra/230Th and 231Pa/235U. These data do not indicate a simple mixing trend between an N-MORB and an enriched component in the 231Pa/235U versus 230Th/238U diagram since the MORBs which do not have the most radiogenic isotope signatures compared with the Azores island basalts have some of the largest (230Th/238U) and 231Pa/235U. Clearly, the dynamics of melting must have played a role in generating larger 230Th and 231Pa excesses beneath the Mid-Atlantic ridge. We infer that this must be due to the absence of a lithospheric lid as larger excesses of 230Th and 231Pa can be generated for longer melting columns. Thus, ridge-hotspot interaction cannot imply a simple transfer of melt from the hotspot to the ridge. The 230Th/238U and 226Ra/230Th data across the Azores plateau shows a maximum for the island of Terceira and mimics the depth anomaly which is thought to result from the hotspot. This trend is also consistent with observations of rare gases (M. Moreira pers. comm.) and suggests that it must be related to the presence of deep material. The U-series trend is the reverse of the trend found in Hawaii by Sims et al. (2000) which was attributed to variations in upwelling rates across the rising plume. This observation can be rationalized in the context of an equilibrium melt transport model (Spiegelman and Elliott, 1993) where U-series disequilibria are sensitive to upwelling rates. For slow upwelling rates such as below the Azores, larger 230Th excesses are predicted in the center of the plume. This suggests that the upwelling rate beneath the center of the plume must be of the order of a few cm per year which is an order of magnitude lower than values estimated for Hawaii. Turner et al. 1997, Chem. Geol. 139, 145-164. Bourdon et al. 1996, Earth Planet. Sci. Lett. 142, 175-189. Pickett et al. 1997, Earth Planet. Sci. Lett. 148, 259-271. Sims et al. 1999, Geochim. Cosmochim. Acta. 63, 4119-4138. Spiegelman and Elliot, 1993, Earth Planet. Sci. Lett., 118, 1-20.

Geochemical investigations by the U.S. Geological Survey on uranium mining, milling, and environmental restoration

USGS Publications Warehouse

Landa, Edward R.; Cravotta, Charles A.; Naftz, David L.; Verplanck, Philip L.; Nordstrom, D. Kirk; Zielinski, Robert A.

2000-01-01

Recent research by the U.S. Geological Survey has characterized contaminant sources and identified important geochemical processes that influence transport of radionuclides from uranium mining and milling wastes. 1) Selective extraction studies indicated that alkaline earth sulfates and hydrous ferric oxides are important hosts of 226Ra in uranium mill tailings. The action of sulfate-reducing and ironreducing bacteria on these phases was shown to enhance release of radium, and this adverse result may temper decisions to dispose of uranium mill tailings in anaerobic environments. 2) Field studies have shown that although surface-applied sewage sludge/wood chip amendments aid in revegetating pyritic spoil, the nitrogen in sludge leachate can enhance pyrite oxidation, acidification of groundwater, and the consequent mobilization of metals and radionuclides. 3) In a U.S. Environmental Protection Agencyfunded study, three permeable reactive barriers consisting of phosphate-rich material, zero-valent iron, or amorphous ferric oxyhydroxide have been installed at an abandoned uranium upgrader facility near Fry Canyon, UT. Preliminary results indicate that each of the permeable reactive barriers is removing the majority of the uranium from the groundwater. 4) Studies on the geochemistry of rare earth elements as analogues for actinides such as uranium and thorium in acid mine drainage environments indicate high mobility under acid-weathering conditions but measurable attenuation associated with iron and aluminum colloid formation. Mass balances from field and laboratory studies are being used to quantify the amount of attenuation. 5) A field study in Colorado demonstrated the use of 234U/238U isotopic ratio measurements to evaluate contamination of shallow groundwater with uranium mill effluent.

TOF-SIMS for Rapid Nuclear Forensics Evaluation of Uranium Oxide Particles

DTIC Science & Technology

2011-03-01

Fraction U-238 nU U metal CRM 112-A NBL Metal Assay and Isotopic .000052458 .0072017 --- .9927458 nUO2 UO2 --- NBL Commercial material...0 .992745 dU U metal CRM 115 NBL Uranium Assay .0000076 .0020291 .0000322 .9979311 dUO2 UO2 --- IBI Labs Commercial material --- .002- .0035...U500* U3O8 CRM U500 NBL Isotopic .005181 .49696 .000755 .49711 U900* U3O8 CRM U900 NBL Isotopic .007777 .90196 .003327 .08693 *Sample

Depleted and natural uranium: chemistry and toxicological effects.

PubMed

Craft, Elena; Abu-Qare, Aquel; Flaherty, Meghan; Garofolo, Melissa; Rincavage, Heather; Abou-Donia, Mohamed

2004-01-01

Depleted uranium (DU) is a by-product from the chemical enrichment of naturally occurring uranium. Natural uranium is comprised of three radioactive isotopes: (238)U, (235)U, and (234)U. This enrichment process reduces the radioactivity of DU to roughly 30% of that of natural uranium. Nonmilitary uses of DU include counterweights in airplanes, shields against radiation in medical radiotherapy units and transport of radioactive isotopes. DU has also been used during wartime in heavy tank armor, armor-piercing bullets, and missiles, due to its desirable chemical properties coupled with its decreased radioactivity. DU weapons are used unreservedly by the armed forces. Chemically and toxicologically, DU behaves similarly to natural uranium metal. Although the effects of DU on human health are not easily discerned, they may be produced by both its chemical and radiological properties. DU can be toxic to many bodily systems, as presented in this review. Most importantly, normal functioning of the kidney, brain, liver, and heart can be affected by DU exposure. Numerous other systems can also be affected by DU exposure, and these are also reviewed. Despite the prevalence of DU usage in many applications, limited data exist regarding the toxicological consequences on human health. This review focuses on the chemistry, pharmacokinetics, and toxicological effects of depleted and natural uranium on several systems in the mammalian body. A section on risk assessment concludes the review.

49 CFR 234.6 - Penalties.

Code of Federal Regulations, 2012 CFR

2012-10-01

... death or injury to persons, or has caused death or injury, a penalty not to exceed $105,000 per... 49 Transportation 4 2012-10-01 2012-10-01 false Penalties. 234.6 Section 234.6 Transportation... SYSTEMS General § 234.6 Penalties. (a) Civil penalty. Any person (an entity of any type covered under 1 U...

49 CFR 234.6 - Penalties.

Code of Federal Regulations, 2014 CFR

2014-10-01

... death or injury to persons, or has caused death or injury, a penalty not to exceed $105,000 per... 49 Transportation 4 2014-10-01 2014-10-01 false Penalties. 234.6 Section 234.6 Transportation... SYSTEMS General § 234.6 Penalties. (a) Civil penalty. Any person (an entity of any type covered under 1 U...

49 CFR 234.6 - Penalties.

Code of Federal Regulations, 2013 CFR

2013-10-01

... death or injury to persons, or has caused death or injury, a penalty not to exceed $105,000 per... 49 Transportation 4 2013-10-01 2013-10-01 false Penalties. 234.6 Section 234.6 Transportation... SYSTEMS General § 234.6 Penalties. (a) Civil penalty. Any person (an entity of any type covered under 1 U...

49 CFR 234.6 - Penalties.

Code of Federal Regulations, 2011 CFR

2011-10-01

... 49 Transportation 4 2011-10-01 2011-10-01 false Penalties. 234.6 Section 234.6 Transportation... TRANSPORTATION GRADE CROSSING SIGNAL SYSTEM SAFETY AND STATE ACTION PLANS General § 234.6 Penalties. (a) Civil penalty. Any person (an entity of any type covered under 1 U.S.C. 1, including but not limited to the...

49 CFR 234.6 - Penalties.

Code of Federal Regulations, 2010 CFR

2010-10-01

... 49 Transportation 4 2010-10-01 2010-10-01 false Penalties. 234.6 Section 234.6 Transportation... TRANSPORTATION GRADE CROSSING SIGNAL SYSTEM SAFETY AND STATE ACTION PLANS General § 234.6 Penalties. (a) Civil penalty. Any person (an entity of any type covered under 1 U.S.C. 1, including but not limited to the...

Transfer Rates of 238U and 232Th for E. globulus, A. mearnsii, H. filipendula and Hazardous Effects of the Usage of Medicinal Plants From Around Gold Mine Dump Environs

PubMed Central

Tshivhase, Victor M.; Njinga, Raymond L.; Mathuthu, Manny; Dlamini, Thulani C.

2015-01-01

Medicinal plant consumption can be a source of human exposure to radioactive elements such as 238U and 232Th, which can lead to internal radiation doses. The uptake of 238U and 232Th from soils to the leaf samples of three different medicinal plant species (Eucalyptus globulus, Acacia mearnsii and Hyparrhenia filipendula) from the purlieu of the Princess gold mine dump, an abandoned contaminated tailings storage site (TSS), located at longitude 27°55′00″E and latitude 26°09′30″S in Davidsonville (Roodepoort, west of Johannesburg, South Africa) was measured. This was done using ICP-MS spectrometry and substantial differences were observed in the soil-plant transfer factor (TF) values between these radionuclides. The plant species E. globulus exhibited the highest uptake of 238U, with an average TF of 3.97, while that of H. filipendula was 0.01 and the lowest TF of 0.15 × 10−2 was measured for A. mearnsii. However, in the case of 232Th, the highest average TF was observed for A. mearnsii (0.29), followed by E. globulus (0.10) and lowest was measured for H. filipendula (0.27 × 10−2). The ratio of TF average value i.e., 238U to 232Th in the soil-plant leaves was 38.05 for E. globulus, 0.01 for A. mearnsii and 4.38 for H. filipendula. PMID:26690462

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

NASA Astrophysics Data System (ADS)

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

2015-06-01

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

238U-230Th dating of chevkinite in high-silica rhyolites from La Primavera and Yellowstone calderas

USGS Publications Warehouse

Vazquez, Jorge A.; Velasco, Noel O.; Schmitt, Axel K.; Bleick, Heather A.; Stelten, Mark E.

2014-01-01

Application of 238U-230Th disequilibrium dating of accessory minerals with contrasting stabilities and compositions can provide a unique perspective on magmatic evolution by placing the thermochemical evolution of magma within the framework of absolute time. Chevkinite, a Th-rich accessory mineral that occurs in peralkaline and metaluminous rhyolites, may be particularly useful as a chronometer of crystallization and differentiation because its composition may reflect the chemical changes of its host melt. Ion microprobe 128U-230Th dating of single chevkinite microphenocrysts from pre- and post-caldera La Primavera, Mexico, rhyolites yields model crystallization ages that are within 10's of k.y. of their corresponding K-Ar ages of ca. 125 ka to 85 ka, while chevkinite microphenocrysts from a post-caldera Yellowstone, USA, rhyolite yield a range of ages from ca. 110 ka to 250 ka, which is indistinguishable from the age distribution of coexisting zircon. Internal chevkinite-zircon isochrons from La Primavera yield Pleistocene ages with ~5% precision due to the nearly two order difference in Th/U between both minerals. Coupling chevkinite 238U-230Th ages and compositional analyses reveals a secular trend of Th/U and rare earth elements recorded in Yellowstone rhyolite, likely reflecting progressive compositional evolution of host magma. The relatively short timescale between chevkinite-zircon crystallization and eruption suggests that crystal-poor rhyolites at La Primavera were erupted shortly after differentiation and/or reheating. These results indicate that 238U-230Th dating of chevkinite via ion microprobe analysis may be used to date crystallization and chemical evolution of silicic magmas.

Calling for a Truce on the Military Divorce Battlefield: A Proposal to Amend the USFSPA

DTIC Science & Technology

2001-04-01

28 Silkwood v. Kerr-McGee Corp., 464 U.S. 238, 248 (1984). 7 preempting domestic relations law, the Supreme Court has held that "state interests...that field is pre-empted." Silkwood v. Kerr-McGee Corp., 464 U.S. 238, 248 (1984). Because Congress has occupied the field of military retirement

Weak e+e- lines from internal pair conversion observed in collisions of 238U with heavy nuclei

NASA Astrophysics Data System (ADS)

Heinz, S.; Berdermann, E.; Heine, F.; Joeres, O.; Kienle, P.; Koenig, I.; Koenig, W.; Kozhuharov, C.; Leinberger, U.; Rhein, M.; Schröter, A.; Tsertos, H.

1998-01-01

We present the results of a Doppler-shift correction to the measured e+e- sum-energy spectra obtained from e+e- coincidence measurements in 238U +206Pb and 238U +181Ta collisions at beam energies close to the Coulomb barrier, using an improved experimental setup at the double-Orange spectrometer of GSI. Internal-Pair-Conversion (IPC) e+e- pairs from discrete nuclear transitions of a moving emitter have been observed following Coulomb excitation of the 1.844 MeV (E1) transition in 206Pb and neutron transfer to the 1.770 MeV (M1) transition in 207Pb. In the collision system 238U +181Ta, IPC transitions were observed from the Ta-like as well as from the U-like nuclei. In all systems the Doppler-shift corrected e+e- sum-energy spectra show weak lines at the energies expected from the corresponding γ ray spectra with cross sections being consistent with the measured excitation cross sections of the γ lines and the theoretically predicted IPC coefficients. No other than IPC e+e- sum-energy lines were found in the measured spectra. The transfer cross sections show a strong dependence on the distance of closest approach (Rmin), thus signaling also a strong dependence on the bombarding energy close to the Coulomb barrier.

On the Search for Nuclear Resonance Fluorescence Signatures of 235U and 238U above 3 MeV

DOE Office of Scientific and Technical Information (OSTI.GOV)

Warren, Glen A.; Caggiano, Joseph A.; Bertozzi, William

Nuclear resonance fluorescence is a physical process that provides an isotope-specific signature that could be used for the identification and characterization of materials. The technique involves the detection of prompt discrete-energy photons emitted from a sample that is exposed to MeV-energy photons. Potential applications of the technique range from detection of high explosives to characterization of special nuclear materials such as 235U. Pacific Northwest National Laboratory and Passport Systems have collaborated to conduct a pair of measurements to search for a nuclear resonance fluorescence response of 235U above 3 MeV and of 238U above 5 MeV using an 8 gmore » sample of highly enriched uranium and a 90 g sample of depleted uranium. No new signatures were observed. The minimum detectable integrated cross section for 235U is presented.« less

On the Search for Nuclear Resonance Fluorescence Signatures of 235U and 238U above 3 MeV

DOE Office of Scientific and Technical Information (OSTI.GOV)

Warren, Glen A.; Caggiano, Joseph A.; Bertozzi, William

Abstract–Nuclear resonance fluorescence is a physical process that provides an isotope-specific signature that could be used for the identification and characterization of materials. The technique involves the detection of prompt discrete-energy photons emitted from a sample that is exposed to photons in the MeV energy range. Potential applications of the technique range from detection of high explosives to characterization of special nuclear materials such as 235U. Pacific Northwest National Laboratory and Passport Systems have collaborated to conduct a a pair of measurements to search for a nuclear resonance fluorescence response of 235U above 3 MeV and of 238U above 5more » MeV using an 8 g sample of highly enriched uranium and a 90 g sample of depleted uranium. No new signatures were observed. The minimum detectable integrated cross section for 235U is presented.« less

Formation ages and evolution of Shergotty and its parent planet from U-Th-Pb systematics

NASA Technical Reports Server (NTRS)

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

1986-01-01

The isotopic composition of Pb from Shergotty, Zagami, and EETA 79001 meteorites was determined for different phases. Using phases with low U-238/Pb-204 ratio, the initial leads of these meteorites were defined. Samples from all three meteorites were shown to have distinct initial leads, and, thus to have evolved from different reservoirs over most of solar system history in a low U-238/Pb-204 environment. It follows that the parent planet of the shergottites has a high Pb-204 concentration relative to U and must also be high in other volatiles. The possibility of the Martian origin of the SNC-type meteorites is discussed.

Analysis of a Uranium Oxide Sample Interdicted in Slovakia (FSC 12-3-1)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borg, Lars E.; Dai, Zurong; Eppich, Gary R.

2014-01-17

We provide a concise summary of analyses of a natural uranium sample seized in Slovakia in November 2007. Results are presented for compound identification, water content, U assay, trace element abundances, trace organic compounds, isotope compositions for U, Pb, Sr and O, and age determination using the 234U – 230Th and 235U – 231Pa chronometers. The sample is a mixture of two common uranium compounds - schoepite and uraninite. The uranium isotope composition is indistinguishable from natural; 236U was not detected. The O, Sr and Pb isotope compositions and trace element abundances are unremarkable. The 234U – 230Th chronometer givesmore » an age of 15.5 years relative to the date of analysis, indicating the sample was produced in January 1997. A comparison of the data for this sample with data in the Uranium Sourcing database failed to find a match, indicating the sample was not produced at a facility represented in the database.« less

Counting neutrons from the spontaneous fission of {sup 238}U using scintillation detectors and mixed field analysers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parker, Helen M. O'D.; Joyce, Malcolm J.; Jones, Ashley

2015-07-01

It is well documented that {sup 238}U decays by spontaneous fission, and that it is the main component of most nuclear fuels. As nuclear fuels are largely classed as Special Nuclear Material (SNM), they have to be fully accounted for by owners and processing facilities. One possible method for verifying declared amounts of SNM is to count the spontaneous neutrons produced from {sup 238}U. Using four EJ-309 liquid scintillation detectors and a mixed field analyser, spontaneous neutrons from 16.4 g of depleted uranium (0.3% enrichment) have been assayed. The assay method shows promising results and this proof of principle willmore » be researched further in order for it to be applied in an industrial setting. (authors)« less

Preliminary study of a radiological survey in an abandoned uranium mining area in Madagascar

NASA Astrophysics Data System (ADS)

N, Rabesiranana; M, Rasolonirina; F, Solonjara A.; Andriambololona., Raoelina; L, Mabit

2010-05-01

The region of Vinaninkarena located in central Madagascar (47°02'40"E, 19°57'17"S), is known to be a high natural radioactive area. Uranium ore was extracted in this region during the 1950s and the early 1960s. In the mid-1960s, mining activities were stopped and the site abandoned. In the meantime, the region, which used to be without any inhabitants, has recently been occupied by new settlers with presumed increase in exposure of the local population to natural ionizing radiation. In order to assess radiological risk, a survey to assess the soil natural radioactivity background was conducted during the year 2004. This study was implemented in the frame of the FADES Project SP99v1b_21 entitled: Assessment of the environmental pollution by multidisciplinary approach, and the International Atomic Energy Agency Technical Cooperation Project MAG 7002 entitled: Effects of air and water pollution on human health. Global Positioning System (GPS) was used to determine the geographical coordinates of the top soil samples (0-15cm) collected. The sampling was performed using a multi integrated scale approach to estimate the spatial variability of the parameters under investigation (U, Th and K) using geo-statistical approach. A total of 205 soil samples was collected in the study site (16 km2). After humidity correction, the samples were sealed in 100 cm3 cylindrical air-tight plastic containers and stored for more than 6 months to reach a secular equilibrium between parents and short-lived progeny (226Ra and progeny, 238U and 234Th). Measurements were performed using a high-resolution HPGe Gamma-detector with a 30% relative efficiency and an energy resolution of 1.8 keV at 1332.5 keV, allowing the determination of the uranium and thorium series and 40K. In case of secular equilibrium, a non-gamma-emitting radionuclide activity was deduced from its gamma emitting progeny. This was the case for 238U (from 234Th), 226Ra (from 214Pb and 214Bi) and 232Th (from 228Ac, 212Pb or 208Tl). Furthermore, in order to assess the radiological effect, the kerma rate in the air at 1 m above ground level was calculated for each sampled points using standard activity-kerma rate conversion coefficients for uranium, thorium series and potassium. Geostatistical interpolation tools (e.g. Inverse Distance Weighting power 2 and Ordinary Kriging) were used to optimize the data set mapping. The measured Potassium-40 activity was 333 Bq kg-1 ± 95% (Mean ± Coefficient of Variation), the Uranium activity was 195 Bq kg-1 ± 53% and the Thorium activity was 139 Bq kg-1 ± 29%. The world average concentrations are reported by the United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR) as 400 Bq kg-1 for 40K, 35 Bq kg-1 for 238U and 30 Bq kg-1 for 232Th. The results show that generally, 40K concentrations in soils of the area are slightly lower than the world average value, whereas uranium and thorium series activities are noticeably higher. On average the kerma rate reaches 143 nGy h-1 with a standard deviation of 41 nGy h-1 and a coefficient of variation of 28%. The information obtained was mapped and the dose exposition was also assessed for the local settlers. Key-words: soil contamination, environmental radioactivity, radioecology, dose exposure.

Kinetically limited weathering at low denudation rates in semi-arid climates

NASA Astrophysics Data System (ADS)

Vanacker, V.; Schoonejans, J.; Opfergelt, S.; Ameijeiras-Marino, Y.; Christl, M.

2016-12-01

On Earth, the Critical Zone supports terrestrial life, being the near-surface environment where interactions between the atmosphere, lithosphere, hydrosphere, and biosphere take place Quantitative understanding of the interaction between mechanical rock breakdown, chemical weathering, and physical erosion is essential for unraveling Earth's biogeochemical cycles. In this study, we explore the role of soil water balance on regulating soil chemical weathering under water deficit regimes. Weathering rates and intensities were evaluated for nine soil profiles located on convex ridge crests of three mountain ranges in the Spanish Betic Cordillera. We present and compare quantitative information on soil weathering, chemical depletion and total denudation that were derived based on geochemical mass balance, 10Be cosmogenic nuclides and U-series disequilibria. Soil production rates determined based on U-series isotopes (238U, 234U, 230Th and 226Ra) are of the same order of magnitude as 10Be-derived denudation rates, suggesting steady state soil thickness, in two out of three sampling sites. The chemical weathering intensities are relatively low (˜5 to 30% of the total denudation of the soil) and negatively correlated with the magnitude of the water deficit in soils. Soil weathering extents increase (nonlinearly) with soil thickness and decrease with increasing surface denudation rates, consistent with kinetically limited or controlled weathering. Our study suggests that soil residence time and water availability limit weathering processes in semi-arid climates, which has not been validated previously with field data. An important implication of this finding is that climatic regimes may strongly regulate soil weathering by modulating soil solute fluxes.

Thorium distributions in high- and low-dust regions and the significance for iron supply

NASA Astrophysics Data System (ADS)

Hayes, Christopher T.; Rosen, Jeffrey; McGee, David; Boyle, Edward A.

2017-02-01

Thorium and uranium isotopes (232Th, 230Th, 238U, and 234U) were investigated to refine their use for estimating mineral dust deposition and Fe delivery to the ocean. U concentrations and isotope ratios were consistent with conservative behavior and can safely be described using published U-salinity relationships and global average seawater isotopic composition. Near Barbados, waters affected by the Amazon outflow contained elevated 232Th. This signals one region where the thorium-dust method is inaccurate because of a confounding continental input. Dissolved 232Th fluxes in this region suggest that Amazonian Fe supply to the adjacent open ocean is much larger than local atmospheric deposition. The colloidal content of dissolved Th south of Bermuda was found to be quite small (2-6%), similar to that found north of Hawaii, despite the order of magnitude higher dust deposition in the Atlantic. This finding supports the assumption that dissolved 232Th and 230Th are scavenged at the same rate despite their different sources and also sheds light on the increase of dissolved 232Th fluxes with integrated depth. Outside the region influenced by Amazon River waters, dissolved 232Th fluxes are compared with Bermudan aerosol Fe deposition to estimate that fractional Th solubility is around 20% in this region. Finally, new dissolved and soluble Fe, Mn, and Cr data from the subtropical North Pacific support the idea that Fe concentrations in the remote ocean are highly buffered, whereas 232Th has a larger dynamic range between high- and low-dust regions.

The age of universe

NASA Astrophysics Data System (ADS)

Ali, Zeeshan

The presence of short-lived isotope Curium-247 in the early Solar System complicates the job of dating the earliest events in the solar nebula. Primitive components in meteorites contain a detailed record of the conditions and processes in the solarnebula, the cloud of dust and gas surrounding the infant Sun. Determining accurately when the first materialsformed re-quires the lead-lead (Pb-Pb) dating method, a method based on the decay of uranium (U) isotopes toPb isotopes. The initial ratio of U-238 to U-235 is critical to determining theages correctly, and many studies have concluded that the ratio is constant for any given age. How-ever, my colleagues at Arizona State University(Frankfurt, Germany), and the Senckenberg Forschungsinstitut und Naturmuseum (also in Frankfurt) and I have found that some calcium-aluminum-rich inclusions (CAIs) in chondritic meteorites deviate from the conventional value for the U-238/U-235 ratio. This could lead to inaccuracies of up to 5 million years in the age of these objects, if no correction is made.Variations in the concentrations of thorium and neodymium with the U-238/U-235 ratio suggest that the ratio may have been lowered by the decay of curium-247, which decays to U-235 with a half-life of 15.6 million years. Curium-247 is created in certain types of energetic supernovae, so its presence suggests that a supernova added material to the pre-solar interstellar cloud between 110 and 140 million years before theSolar System began to form.

A Complication in Determining the Precise Age of the Solar System

NASA Astrophysics Data System (ADS)

Brennecka, G. A.

2010-01-01

Primitive components in meteorites contain a detailed record of the conditions and processes in the solar nebula, the cloud of dust and gas surrounding the infant Sun. Determining accurately when the first materials formed requires the lead-lead (Pb-Pb) dating method, a method based on the decay of uranium (U) isotopes to Pb isotopes. The initial ratio of U-238 to U-235 is critical to determining the ages correctly, and many studies have concluded that the ratio is constant for any given age. However, my colleagues at Arizona State University, Institut fur Geowissenschaften, Goethe-Universitat (Frankfurt, Germany), and the Senckenberg Forschungsinstitut und Naturmuseum (also in Frankfurt) and I have found that some calcium-aluminum-rich inclusions (CAIs) in chondritic meteorites deviate from the conventional value for the U-238/U-235 ratio. This could lead to inaccuracies of up to 5 million years in the age of these objects, if no correction is made. Variations in the concentrations of thorium and neodymium with the U-238/U-235 ratio suggest that the ratio may have been lowered by the decay of curium-247, which decays to U-235 with a half-life of 15.6 million years. Curium-247 is created in certain types of energetic supernovae, so its presence suggests that a supernova added material to the pre-solar interstellar cloud between 110 and 140 million years before the Solar System began to form.

Student Flow Simulation for the Consolidated Navy Electronic Warfare School.

DTIC Science & Technology

1982-07-01

WLR-1 201 202 203 204 205 USN 6YO AN/SLQ-32 206 207 208 209 210 USN 6YO AN/SLQ-17 211 212 213 214 215 JSN 6YO AN/WLR-8 216 217 218 219 220 uSN 4YO AN...WLR-I 221 222 2?3 224 225 JSN 4YO AN/SLQ-32 226 227 228 229 230 UrN 4YO AN/SLQ-17 231 232 233 234 235 USN 4YO AN/WLR-8 236 237 238 2 9 240 JSN 3X6 AN...USN 6YO 1 ASSIGN node ASS3 (after CDP 3C) USN 4YO 2 GOON node N3 USN 3X6 3 GOON node N3 USN Late Conv. 4 GOON node N3 Fit. Returnee 6 Introduced in the

Distribution of uranium and thorium in groundwater of arid climate region

NASA Astrophysics Data System (ADS)

Murad, Ahmed; Alshamsi, Dalal; Aldahan, Ala; Hou, Xiaolin

2014-05-01

Uranium, thorium and their decay products are the most common radionuclides in groundwater in addition to potassium-40. Once groundwater is used for drinking, domestic and irrigation purposes, the radionuclides will then pose environmental and health related hazard originating from radioactivity and toxicity. In the investigation presented here, assessment of 238U, 235U and 232Th concentrations in groundwater across of the United Arab Emirates (UAE) is evaluated in terms of quality and sources. The region is dominated by arid climate conditions and radioactivity assessment of groundwater is essential for safe use of groundwater. Furthermore, the results were linked to data from other arid regions and worldwide. Groundwater samples (total dissolved solids,TDS, 142.5 mg L-1 to 12770 mg L-1) from 67 different wells were collected across geomorphologically different areas and most of the wells are actively used for agriculture. The aquifers are recent sand dunes, Quaternary (3 million years to present) sediments, and older carbonate rocks (230-10 million years). The 235U, 238U and 232Th measurements were carried out using ICP-MS system equipped with an Xt-skimmer cone and a concentric nebulizer under hot plasma conditions. Concentrations of 235U, 238U and 232Th range at (0.125-508.4) ng L-1, (25.81-69237) ng L-1 and (0.236-2529) ng L-1, respectively. Apparently, most 235U, 238U, 232Th concentrations in the sampled groundwater are below the WHO proposed permissible level of 60000 ng/L for total uranium (1 Bq L-1 for 235U and 10 Bq L-1 for 238U) and 5000 ng L-1 (1Bq L-1) for 232Th. A few samples show high concentrations of uranium that are associated with high TDS values and occur within interbedded limestones and shales aquifer. Comparison with worldwide groundwater data suggests that 238U concentration is highest in the arid regions groundwater where the recharge to aquifers is relatively low. The situation for 232Th concentrations seems less affected by climatic conditions, most likely is related to its less solubility in water compared to uranium. We calculated the accumulated TU and 232Th concentration in the irrigation water annually to estimate the cumulative concentrations after twenty years on specific agricultural areas. The TU and 232Th are expected not to reach more than 1.14 x 10-3 g (1.14 mg) and 4.32 x 10-6 g (4.32 μg) respectively after twenty years if the daily irrigation is at its maximum amount (10 m3). Despite these obtained values of concentrations in irrigation water, the transfer of uranium and thorium into crop is not readily and it is expected that only a tiny fraction of the element end into the body. However, further research is needed to quantify the dietary exposures in the UAE with detailed data from crops and consumers.

Radium and uranium levels in vegetables grown using different farming management systems.

PubMed

Lauria, D C; Ribeiro, F C A; Conti, C C; Loureiro, F A

2009-02-01

Vegetables grown with phosphate fertilizer (conventional management), with bovine manure fertilization (organic management) and in a mineral nutrient solution (hydroponic) were analyzed and the concentrations of (238)U, (226)Ra and (228)Ra in lettuce, carrots, and beans were compared. Lettuce from hydroponic farming system showed the lowest concentration of radionuclides 0.51 for (226)Ra, 0.55 for (228)Ra and 0.24 for (238)U (Bq kg(-1) dry). Vegetables from organically and conventionally grown farming systems showed no differences in the concentration of radium and uranium. Relationships between uranium content in plants and exchangeable Ca and Mg in soil were found, whereas Ra in vegetables was inversely correlated to the cation exchange capacity of soil, leading to the assumption that by supplying carbonate and cations to soil, liming may cause an increase of U and a decrease of radium uptake by plants. The soil to plant transfer varied from 10(-4) to 10(-2) for (238)U and from 10(-2) to 10(-1) for (228)Ra.

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

NASA Astrophysics Data System (ADS)

Duke, Dana

2015-10-01

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

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.

Mass and abundance 236U sensitivities at CIRCE

NASA Astrophysics Data System (ADS)

De Cesare, M.; De Cesare, N.; D'Onofrio, A.; Fifield, L. K.; Gialanella, L.; Terrasi, F.

2015-10-01

The actinides (e.g. 236U and xPu isotopes) are present in environmental samples at the ultra trace level since atmospheric tests of NWs (Nuclear Weapons) performed in the past, deliberate dumping of nuclear waste, nuclear fuel reprocessing, on a large scale and operation of NPPs (Nuclear Power Plants) on a small scale have led to the release of a wide range of radioactive nuclides in the environment. Their detection requires the most sensitive AMS (Accelerator Mass Spectrometry) techniques and at the Center for Isotopic Research on Cultural and Environmental heritage (CIRCE) in Caserta, Italy, an upgraded actinide AMS system, based on a 3-MV pelletron tandem accelerator, has been operated. In this paper the progress made in order to push the 236U mass sensitivity and 236U/238U isotopic ratio down to the natural levels is reported. A uranium contamination mass of about 0.05 μg and a 236U/238U isotopic ratio sensitivities at the level of 3.2 × 10-13 are presently achievable.

Radionuclide Concentrations in Soils and Vegetation at Low-Level Radioactive Waste Disposal Area G during the 1997 Growing Season

DOE Office of Scientific and Technical Information (OSTI.GOV)

L. Naranjo, Jr.; P. R. Fresquez; R. J. Wechsler

1998-08-01

Soil and overstory and understory vegetation (washed and unwashed) collected at eight locations within and around Area G-a low-level radioactive solid-waste disposal facility at Los Alamos National Laboratory-were analyzed for 3H, 238Pu, 239Pu, 137CS, 234U, 235U, 228AC, Be, 214Bi, 60Co, 40& 54Mn, 22Na, 214Pb and 208Tl. In general, most radionuclide concentrations, with the exception of 3Ef and ~9Pu, in soils and overstory and understory vegetation collected from within and around Area G were within upper (95'%) level background concentrations. Although 3H concentrations in vegetation from most sites were significantly higher than background (>2 pCi mL-l), concentrations decreased markedly in comparisonmore » to last year's results. The highest `H concentration in vegetation was detected from a juniper tree that was growing over tritium shaft /+150; it contained 530,000 pCi 3H mL-l. Also, as in the pas~ the transuranic waste pad area contained the highest levels of 239Pu in soils and in understory vegetation as compared to other areas at Area G.« less

Plant uptake of 238U, 235U, 232Th, 226Ra, 210Pb and 40K from a coal ash and slag disposal site and control soil under field conditions: A preliminary study.

PubMed

Skoko, Božena; Marović, Gordana; Babić, Dinko; Šoštarić, Marko; Jukić, Mirela

2017-06-01

The aim of this study was to investigate the uptake of 238 U, 235 U, 232 Th, 226 Ra, 210 Pb and 40 K by plants that grow on a coal ash and slag disposal site known for its higher content of naturally occurring radionuclides. Plant species that were sampled are common for the Mediterranean flora and can be divided as follows: grasses & herbs, shrubs and trees. To compare the activity concentrations and the resultant concentration ratios of the disposal site with those in natural conditions, we used control data specific for the research area, obtained for plants growing on untreated natural soil. Radionuclide activity concentrations were determined by high resolution gamma-ray spectrometry. Media parameters (pH, electrical conductivity and organic matter content) were also analysed. We confirmed significantly higher activity concentrations of 238 U, 235 U, 226 Ra and 210 Pb in ash and slag compared to control soil. However, a significant increase in the radionuclide activity concentration in the disposal site's vegetation was observed only for 226 Ra. On the contrary, a significantly smaller activity concentration of 40 K in ash and slag had no impact on its activity concentration in plant samples. The calculated plant uptake of 238 U, 235 U, 226 Ra and 210 Pb is significantly smaller in comparison with the uptake at the control site, while it is vice versa for 40 K. No significant difference was observed between the disposal site and the control site's plant uptake of 232 Th. These results can be the foundation for further radioecological assessment of this disposal site but also, globally, they can contribute to a better understanding of nature and long-term management of such disposal sites. Copyright © 2017 Elsevier Ltd. All rights reserved.

U-series dating of Lake Nyos maar basalts, Cameroon (West Africa): Implications for potential hazards on the Lake Nyos dam

NASA Astrophysics Data System (ADS)

Aka, Festus T.; Yokoyama, Tetsuya; Kusakabe, Minoru; Nakamura, Eizo; Tanyileke, Gregory; Ateba, Bekoa; Ngako, Vincent; Nnange, Joseph; Hell, Joseph

2008-09-01

From previously published 14C and K-Ar data, the age of formation of Lake Nyos maar in Cameroon is still in dispute. Lake Nyos exploded in 1986, releasing CO 2 that killed 1750 people and over 3000 cattle. Here we report results of the first measurements of major elements, trace elements and U-series disequilibria in ten basanites/trachy-basalts and two olivine tholeiites from Lake Nyos. It is the first time tholeiites are described in Lake Nyos. But for the tholeiites which are in 238U- 230Th equilibrium, all the other samples possess 238U- 230Th disequilibrium with 15 to 28% enrichment of 230Th over 238U. The ( 226Ra/ 230Th) activity ratios of these samples indicate small (2 to 4%) but significant 226Ra excesses. U-Th systematics and evidence from oxygen isotopes of the basalts and Lake Nyos granitic quartz separates show that the U-series disequilibria in these samples are source-based and not due to crustal contamination or post-eruptive alteration. Enrichment of 230Th is strong prima facie evidence that Lake Nyos is younger than 350 ka. The 230Th- 226Ra age of Nyos samples calculated with the ( 226Ra/ 230Th) ratio for zero-age Mt. Cameroon samples is 3.7 ± 0.5 ka, although this is a lower limit as the actual age is estimated to be older than 5 ka, based on the measured mean 230Th/ 238U activity ratio. The general stability of the Lake Nyos pyroclastic dam is a cause for concern, but judging from its 230Th- 226Ra formation age, we do not think that in the absence of a big rock fall or landslide into the lake, a big earthquake or volcanic eruption close to the lake, collapse of the dam from erosion alone is as imminent and alarming as has been suggested.

Separation of actinides from lanthanides utilizing molten salt electrorefining

DOE Office of Scientific and Technical Information (OSTI.GOV)

Grimmett, D.L.; Fusselman, S.P.; Roy, J.J.

1996-10-01

TRUMP-S (TRansUranic Management through Pyropartitioning Separation) is a pyrochemical process being developed to separate actinides form fission products in nuclear waste. A key process step involving molten salt electrorefining to separate actinides from lanthanides has been studied on a laboratory scale. Electrorefining of U, Np, Pu, Am, and lanthanide mixtures from molten cadmium at 450 C to a solid cathode utilizing a molten chloride electrolyte resulted in > 99% removal of actinides from the molten cadmium and salt phases. Removal of the last few percent of actinides is accompanied by lowered cathodic current efficiency and some lanthanide codeposition. Actinide/lanthanide separationmore » ratios on the cathode are ordered U > Np > Pu > Am and are consistent with predictions based on equilibrium potentials.« less

Isotopic fission-fragment distributions of 238U, 239Np, 240Pu, 244Cm, and 250Cf produced through inelastic scattering, transfer, and fusion reactions in inverse kinematics

NASA Astrophysics Data System (ADS)

Ramos, D.; Caamaño, M.; Farget, F.; Rodríguez-Tajes, C.; Audouin, L.; Benlliure, J.; Casarejos, E.; Clement, E.; Cortina, D.; Delaune, O.; Derkx, X.; Dijon, A.; Doré, D.; Fernández-Domínguez, B.; de France, G.; Heinz, A.; Jacquot, B.; Navin, A.; Paradela, C.; Rejmund, M.; Roger, T.; Salsac, M.-D.; Schmitt, C.

2018-05-01

Transfer- and fusion-induced fission in inverse kinematics has proved to be a powerful tool to investigate nuclear fission, widening information on the fission fragments and access to unstable fissioning systems with respect to other experimental approaches. An experimental campaign is being carried out at GANIL with this technique since 2008. In these experiments, a beam of 238U, accelerated to 6.1 MeV/u, impinges on a 12C target. Fissioning systems from U to Cf are populated through inelastic scattering, transfer, and fusion reactions, with excitation energies that range from a few MeV up to 46 MeV. The use of inverse kinematics, the SPIDER telescope, and the VAMOS spectrometer allow the characterization of the fissioning system in terms of mass, nuclear charge, and excitation energy, and the isotopic identification of the full fragment distribution. This work reports on new data from the second experiment of the campaign on fission-fragment yields of the heavy actinides 238U, 239Np, 240Pu, 244Cm, and 250Cf, which are of interest from both fundamental and application points of view.

Analysis of 238U, 232Th, 222Rn, and 220Rn in different medical drug preparations by using CR-39 and LR-115 typE II SSNTDs and resulting radiation doses to adult patients.

PubMed

Misdaq, M A; Karime, M

2009-01-01

Uranium (238U) and thorium (232Th) concentrations as well as radon (222Rn) and thoron (220Rn) alpha activities per unit volume have been measured inside 18 medical drugs (4 liquid and 14 solid materials), widely prescribed by doctors to the Moroccan adult patients, by using CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs). The measured 238U, 232Th, 222Rn, and 220Rn concentrations ranged from (4.7 +/- 0.1) mBq L-1 to (14.3 +/- 0.7) mBq L-1, (0.32 +/- 0.02) mBq L-1 to (2.7 +/- 0.2) mBq L-1, (4.7 +/- 0.2) Bq L-1 to (14.3 +/- 0.7) Bq L-1, and (0.32 +/- 0.02) Bq L-1 to (2.7 +/- 0.2) Bq L-1 for the medical drug samples studied, respectively. These radionuclides were also measured inside the preparations of the solid medical drugs studied. The influence of the drinking water nature and pollution on the concentrations of these radionuclides inside the considered medical drug preparations was investigated. Annual committed equivalent doses due to 238U, 232Th, and 222Rn were evaluated in the human body compartments of adult patients from the ingestion of the medical drug preparations studied. The maximum total committed effective dose due to 238U, 232Th, and 222Rn from the ingestion of the studied medical drug preparations, prepared from unpolluted waters, by adult patients was found equal to 1.44 microSv y.

Fission fragment yields and total kinetic energy release in neutron-induced fission of235,238U,and239Pu

NASA Astrophysics Data System (ADS)

Tovesson, F.; Duke, D.; Geppert-Kleinrath, V.; Manning, B.; Mayorov, D.; Mosby, S.; Schmitt, K.

2018-03-01

Different aspects of the nuclear fission process have been studied at Los Alamos Neutron Science Center (LANSCE) using various instruments and experimental techniques. Properties of the fragments emitted in fission have been investigated using Frisch-grid ionization chambers, a Time Projection Chamber (TPC), and the SPIDER instrument which employs the 2v-2E method. These instruments and experimental techniques have been used to determine fission product mass yields, the energy dependent total kinetic energy (TKE) release, and anisotropy in neutron-induced fission of U-235, U-238 and Pu-239.

Fission-fragment total kinetic energy and mass yields for neutron-induced fission of 235U and 238U with En =200 keV - 30 MeV

NASA Astrophysics Data System (ADS)

Duke, D. L.; Tovesson, F.; Brys, T.; Geppert-Kleinrath, V.; Hambsch, F.-J.; Laptev, A.; Meharchand, R.; Manning, B.; Mayorov, D.; Meierbachtol, K.; Mosby, S.; Perdue, B.; Richman, D.; Shields, D.; Vidali, M.

2017-09-01

The average Total Kinetic Energy (TKE) release and fission-fragment yields in neutron-induced fission of 235U and 238U was measured using a Frisch-gridded ionization chamber. These observables are important nuclear data quantites that are relevant to applications and for informing the next generation of fission models. The measurements were performed a the Los Alamos Neutron Science Center and cover En = 200 keV - 30 MeV. The double-energy (2E) method was used to determine the fission-fragment yields and two methods of correcting for prompt-neutron emission were explored. The results of this study are correlated mass and TKE data.

The positron peak puzzle - Recent results from APEX

DOE PAGES

Ahmad, I; Austin, SM; Back, BB; ...

1996-01-01

Results are presented from a new experiment, APEX, designed to study the previously reported sharp lines in sum-energy spectra of positrons and electrons produced in collisions of very heavy ions. Data have been collected for 238U + 181Ta and 238U + 232Th. No evidence is found for narrow structures similar to those previously reported. For the specific case of the isolated decay of a neutral particle of mass 1.4–2.1 MeV/c 2, the upper limits on cross sections obtained are significantly less than previously reported. Data are also presented for internal pair conversion in 206Pb. These results are used to setmore » limits for the possible contribution to the pair yield of a 1780 keV transition in 238U observed in heavy-ion gamma-ray coincidence measurements.« less

Delayed recovery from the end-Triassic extinction due to an increase in the extent of ocean anoxia

NASA Astrophysics Data System (ADS)

Jost, A. B.; Bachan, A.; van de Schootbrugge, B.; Lau, K. V.; Weaver, K. L.; Maher, K.; Payne, J.

2015-12-01

The end-Triassic mass extinction was likely triggered by a rapid rise in pCO2 associated with the emplacement of the Central Atlantic Magmatic Province (CAMP) ca. 201 Ma. Shallow-marine anoxia has long been hypothesized to have caused the extinction and/or delayed the recovery of marine life. However, due to a lack of proxy data, the effects of CAMP emplacement on seawater chemistry remain poorly constrained. Local proxies for anoxia may not reflect widespread ocean redox conditions. However, coupled records of U concentration and isotopic composition (δ238U) in CaCO3 sediments precipitated beneath well-oxygenated bottom waters can potentially serve as a proxy for the global extent of anoxia due to fractionation of U during reduction and associated imbalances in the marine U cycle due to redox changes. We measured δ238U and Th/U values in shallow marine limestones from two stratigraphic sections in the Lombardy Basin, northern Italy, spanning over 400 m, to quantify the change in the extent of ocean anoxia during the end-Triassic extinction. We observe a ca. 0.6‰ negative excursion in δ238U beginning in the lowermost Jurassic, coeval with the onset of the negative δ13C excursion and persisting for the duration of subsequent high δ13C values in the lower-middle Hettangian (earliest Jurassic). Th/U values are generally low at the T/J boundary, peak near the nadir of the δ238U excursion, and steadily return to pre-event values by the end of the measured section. Using a numerical model of the U cycle, we demonstrate that this excursion corresponds to a thirty-fold increase in the extent of anoxia worldwide and a simultaneous increase in the riverine U flux, consistent with increased weathering and eutrophication following massive CO2 injection from CAMP volcanism. Scenarios involving an increase in marine anoxia would also predict higher rates of organic C burial, explaining the large protracted positive δ13C excursion in the lower-mid Hettangian. Recovery of marine fauna, particularly reef builders, was delayed until the late Hettangian, suggesting that environmental conditions were unfavorable for >1 My after the extinction. Uranium isotope data provide strong support for the hypothesis that persistent ocean anoxia inhibited biotic recovery throughout this interval.

Interpolated mapping and investigation of environmental radioactivity levels in soils and mushrooms in the Middle Black Sea Region of Turkey.

PubMed

Türkekul, İbrahim; Yeşilkanat, Cafer Mert; Ciriş, Ali; Kölemen, Uğur; Çevik, Uğur

2018-06-01

The activity concentration of natural ( 238 U, 232 Th, and 40 K) and artificial ( 137 Cs) radionuclides was determined in 50 samples (obtained from the same station) from various species of mushrooms and soil collected from the Middle Black Sea Region (Turkey). The activities of 238 U, 232 Th, 40 K, and 137 Cs were found as 84 ± 16, 45 ± 14, 570 ± 28, and 64 ± 6 Bq kg -1 (dry weight), respectively, in the mushroom samples and as 51 ± 6, 41 ± 6, 201 ± 11, and 44 ± 4 Bq kg -1 , respectively, in the soil samples for the entire area of study. The results of all radionuclide activity measurements, except those of 238 U and 232 Th in the mushroom samples, are consistent with previous studies. In the soil samples, the mean values of 238 U and 232 Th are above the world mean, and the activity mean of 40 K is below the world mean. Finally, the activity estimation was made with both the soil and mushroom samples for unmeasured points within the study area by using the ordinary kriging method. Radiological distribution maps were generated.

Estimation of Groundwater Radon in North Carolina Using Land Use Regression and Bayesian Maximum Entropy.

PubMed

Messier, Kyle P; Campbell, Ted; Bradley, Philip J; Serre, Marc L

2015-08-18

Radon ((222)Rn) is a naturally occurring chemically inert, colorless, and odorless radioactive gas produced from the decay of uranium ((238)U), which is ubiquitous in rocks and soils worldwide. Exposure to (222)Rn is likely the second leading cause of lung cancer after cigarette smoking via inhalation; however, exposure through untreated groundwater is also a contributing factor to both inhalation and ingestion routes. A land use regression (LUR) model for groundwater (222)Rn with anisotropic geological and (238)U based explanatory variables is developed, which helps elucidate the factors contributing to elevated (222)Rn across North Carolina. The LUR is also integrated into the Bayesian Maximum Entropy (BME) geostatistical framework to increase accuracy and produce a point-level LUR-BME model of groundwater (222)Rn across North Carolina including prediction uncertainty. The LUR-BME model of groundwater (222)Rn results in a leave-one out cross-validation r(2) of 0.46 (Pearson correlation coefficient = 0.68), effectively predicting within the spatial covariance range. Modeled results of (222)Rn concentrations show variability among intrusive felsic geological formations likely due to average bedrock (238)U defined on the basis of overlying stream-sediment (238)U concentrations that is a widely distributed consistently analyzed point-source data.

S/sub n/ analysis of the TRX metal lattices with ENDF/B version III data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wheeler, F.J.; Pearlstein, S.

1975-03-01

Two critical assemblies, designated as thermal-reactor benchmarks TRX-1 and TRX-2 for ENDF/B data testing, were analyzed using the one-dimensional S/sub n/-theory code SCAMP. The two assemblies were simple lattices of aluminum-clad, uranium-metal fuel rods in triangular arrays with D$sub 2$O as moderator and reflector. The fuel was low-enriched (1.3 percent $sup 235$U), 0.387-inch in diameter and had an active height of 48 inches. The volume ratio of water to uranium was 2.35 for the TRX-1 lattice and 4.02 for TRX-2. Full-core S/sub n/ calculations based on Version III data were performed for these assemblies and the results obtained were comparedmore » with the measured values of the multiplication factors, the ratio of epithermal-to-thermal neutron capture in $sup 238$U, the ratio of epithermal-to-thermal fission in $sup 235$U, the ratio of $sup 238$U fission to $sup 235$U fission, and the ratio of capture in $sup 238$U to fission in $sup 235$U. Reaction rates were obtained from a central region of the full- core problems. Multigroup cross sections for the reactor calculation were obtained from S/sub n/ cell calculations with resonance self-shielding calculated using the RABBLE treatment. The results of the analyses are generally consistent with results obtained by other investigators. (auth)« less

Abrupt global-ocean anoxia during the Late Ordovician-early Silurian detected using uranium isotopes of marine carbonates.

PubMed

Bartlett, Rick; Elrick, Maya; Wheeley, James R; Polyak, Victor; Desrochers, André; Asmerom, Yemane

2018-05-21

Widespread marine anoxia is hypothesized as the trigger for the second pulse of the Late Ordovician (Hirnantian) mass extinction based on lithologic and geochemical proxies that record local bottom waters or porewaters. We test the anoxia hypothesis using δ 238 U values of marine limestones as a global seawater redox proxy. The δ 238 U trends at Anticosti Island, Canada, document an abrupt late Hirnantian ∼0.3‰ negative shift continuing through the early Silurian indicating more reducing seawater conditions. The lack of observed anoxic facies and no covariance among δ 238 U values and other local redox proxies suggests that the δ 238 U trends represent a global-ocean redox record. The Hirnantian ocean anoxic event (HOAE) onset is coincident with the extinction pulse indicating its importance in triggering it. Anoxia initiated during high sea levels before peak Hirnantian glaciation, and continued into the subsequent lowstand and early Silurian deglacial eustatic rise, implying that major climatic and eustatic changes had little effect on global-ocean redox conditions. The HOAE occurred during a global δ 13 C positive excursion, but lasted longer indicating that controls on the C budget were partially decoupled from global-ocean redox trends. U cycle modeling suggests that there was a ∼15% increase in anoxic seafloor area and ∼80% of seawater U was sequestered into anoxic sediments during the HOAE. Unlike other ocean anoxic events (OAE), the HOAE occurred during peak and waning icehouse conditions rather than during greenhouse climates. We interpret that anoxia was driven by global cooling, which reorganized thermohaline circulation, decreased deep-ocean ventilation, enhanced nutrient fluxes, stimulated productivity, which lead to expanded oxygen minimum zones. Copyright © 2018 the Author(s). Published by PNAS.

Nuclear energy release from fragmentation

NASA Astrophysics Data System (ADS)

Li, Cheng; Souza, S. R.; Tsang, M. B.; Zhang, Feng-Shou

2016-08-01

It is well known that binary fission occurs with positive energy gain. In this article we examine the energetics of splitting uranium and thorium isotopes into various numbers of fragments (from two to eight) with nearly equal size. We find that the energy released by splitting 230,232Th and 235,238U into three equal size fragments is largest. The statistical multifragmentation model (SMM) is applied to calculate the probability of different breakup channels for excited nuclei. By weighing the probability distributions of fragment multiplicity at different excitation energies, we find the peaks of energy release for 230,232Th and 235,238U are around 0.7-0.75 MeV/u at excitation energy between 1.2 and 2 MeV/u in the primary breakup process. Taking into account the secondary de-excitation processes of primary fragments with the GEMINI code, these energy peaks fall to about 0.45 MeV/u.

Neutrons as Party Animals: An Analogy for Understanding Heavy-Element Fissility

NASA Astrophysics Data System (ADS)

Reed, B. Cameron

2012-12-01

I teach a general education class on the history of nuclear physics and the Manhattan Project. About halfway through the course we come to the discovery of fission and Niels Bohr's insight that it is the rare isotope of uranium, U-235, which fissions under slow-neutron bombardment as opposed to the much more common U-238 isotope. As an "explanation" of the differing responses of the two isotopes to bombarding neutrons, I use the known (measured) masses of the various isotopes involved to compute the energies released upon neutron capture and then compare them to the fission barriers of the "compound" nuclei so formed (U-236 and U-239). The energy released in the (neutron + U-235) reaction exceeds the fission barrier by about one million electron-volts (1 MeV), while that for the (neutron + U-238) case falls about 1.6 MeV short. (The fission barriers are respectively about 5.7 and 6.5 MeV.)

Marine anoxia and delayed Earth system recovery after the end-Permian extinction

PubMed Central

Lau, Kimberly V.; Maher, Kate; Altiner, Demir; Kelley, Brian M.; Kump, Lee R.; Lehrmann, Daniel J.; Silva-Tamayo, Juan Carlos; Weaver, Karrie L.; Yu, Meiyi; Payne, Jonathan L.

2016-01-01

Delayed Earth system recovery following the end-Permian mass extinction is often attributed to severe ocean anoxia. However, the extent and duration of Early Triassic anoxia remains poorly constrained. Here we use paired records of uranium concentrations ([U]) and 238U/235U isotopic compositions (δ238U) of Upper Permian−Upper Triassic marine limestones from China and Turkey to quantify variations in global seafloor redox conditions. We observe abrupt decreases in [U] and δ238U across the end-Permian extinction horizon, from ∼3 ppm and −0.15‰ to ∼0.3 ppm and −0.77‰, followed by a gradual return to preextinction values over the subsequent 5 million years. These trends imply a factor of 100 increase in the extent of seafloor anoxia and suggest the presence of a shallow oxygen minimum zone (OMZ) that inhibited the recovery of benthic animal diversity and marine ecosystem function. We hypothesize that in the Early Triassic oceans—characterized by prolonged shallow anoxia that may have impinged onto continental shelves—global biogeochemical cycles and marine ecosystem structure became more sensitive to variation in the position of the OMZ. Under this hypothesis, the Middle Triassic decline in bottom water anoxia, stabilization of biogeochemical cycles, and diversification of marine animals together reflect the development of a deeper and less extensive OMZ, which regulated Earth system recovery following the end-Permian catastrophe. PMID:26884155

Marine anoxia and delayed Earth system recovery after the end-Permian extinction.

PubMed

Lau, Kimberly V; Maher, Kate; Altiner, Demir; Kelley, Brian M; Kump, Lee R; Lehrmann, Daniel J; Silva-Tamayo, Juan Carlos; Weaver, Karrie L; Yu, Meiyi; Payne, Jonathan L

2016-03-01

Delayed Earth system recovery following the end-Permian mass extinction is often attributed to severe ocean anoxia. However, the extent and duration of Early Triassic anoxia remains poorly constrained. Here we use paired records of uranium concentrations ([U]) and (238)U/(235)U isotopic compositions (δ(238)U) of Upper Permian-Upper Triassic marine limestones from China and Turkey to quantify variations in global seafloor redox conditions. We observe abrupt decreases in [U] and δ(238)U across the end-Permian extinction horizon, from ∼3 ppm and -0.15‰ to ∼0.3 ppm and -0.77‰, followed by a gradual return to preextinction values over the subsequent 5 million years. These trends imply a factor of 100 increase in the extent of seafloor anoxia and suggest the presence of a shallow oxygen minimum zone (OMZ) that inhibited the recovery of benthic animal diversity and marine ecosystem function. We hypothesize that in the Early Triassic oceans-characterized by prolonged shallow anoxia that may have impinged onto continental shelves-global biogeochemical cycles and marine ecosystem structure became more sensitive to variation in the position of the OMZ. Under this hypothesis, the Middle Triassic decline in bottom water anoxia, stabilization of biogeochemical cycles, and diversification of marine animals together reflect the development of a deeper and less extensive OMZ, which regulated Earth system recovery following the end-Permian catastrophe.

From mantle to ash cloud: quantifying magma generation, ascent, and degassing rates at Kilauea during short-lived explosive episodes using short-lived U-series radionuclide disequilibria

NASA Astrophysics Data System (ADS)

Girard, G.; Reagan, M. K.; Sims, K. W.; Garcia, M. O.; Pietruszka, A. J.; Thornber, C. R.

2012-12-01

We analyzed for 238U-series isotopes lava, scoria and ash samples erupted from Kilauea volcano, Hawai'i between 1982 and 2008, in order to investigate processes and timescales of magma generation in the mantle, magma ascent through the crust, and eruption. Timescales of degassing during steady-state lava flow activity occurring in Kilauea East Rift Zone and short-lived explosive episodes that occurred in both the East Rift Zone (Pu'u 'O'o vent opening in 1983 and episode 54 at Nāpau crater in January 1997) and on the summit (Halema'uma'u crater eruptions in March 2008) are compared and contrasted. All samples were found to have small but variable 230Th and 226Ra activity excesses over 238U and 230Th, respectively, with (230Th/238U) ratios ranging from 1.00 to 1.13 and (226Ra/230Th) ratios ranging from 1.03 to 1.17. These two variable isotopic disequilibria may reflect local heterogeneities in the mantle underneath Kilauea, with sources in relatively primitive mantle with (238U)-(230Th)-(226Ra) in secular equilibrium and in recently (< 8000 years) depleted mantle with (230Th) and (226Ra) deficits over parent nuclides. In this model, both types of mantle melt to generate Kilauea magmas and subsequently mix in variable proportions. Samples from the brief explosive episodes span the entire composition range, suggesting that they were fed by heterogeneous magma batches which did not homogenize during ascent from the mantle. (210Pb/226Ra) ratios range from 0.75 to 1.00. The lack of correlation between (210Pb/226Ra) and (226Ra/230Th) or (230Th/238U), and the rapid return to secular equilibrium of 210Pb (< 100 years) suggest a fractionation process distinct from and subsequent to the Ra-Th-U fractionation inherited from mantle melting. We hypothesize that 210Pb deficits originate from 222Rn degassing during magma ascent, and estimate magma ascent from lower crust to surface to take place in a maximum of ~ 7 years for the lava flow samples. Products from the explosive episodes have ratios from ~ 0.75 to near equilibrium, suggesting that they comprise of a mix of young melts and degassed magmas which were stored in the shallow volcanic edifice for a few decades, in agreement with existing petrologic models.

Analysis on fuel breeding capability of FBR core region based on minor actinide recycling doping

DOE Office of Scientific and Technical Information (OSTI.GOV)

Permana, Sidik; Novitrian,; Waris, Abdul

Nuclear fuel breeding based on the capability of fuel conversion capability can be achieved by conversion ratio of some fertile materials into fissile materials during nuclear reaction processes such as main fissile materials of U-233, U-235, Pu-239 and Pu-241 and for fertile materials of Th-232, U-238, and Pu-240 as well as Pu-238. Minor actinide (MA) loading option which consists of neptunium, americium and curium will gives some additional contribution from converted MA into plutonium such as conversion Np-237 into Pu-238 and it's produced Pu-238 converts to Pu-239 via neutron capture. Increasing composition of Pu-238 can be used to produce fissilemore » material of Pu-239 as additional contribution. Trans-uranium (TRU) fuel (Mixed fuel loading of MOX (U-Pu) and MA composition) and mixed oxide (MOX) fuel compositions are analyzed for comparative analysis in order to show the effect of MA to the plutonium productions in core in term of reactor criticality condition and fuel breeding capability. In the present study, neptunium (Np) nuclide is used as a representative of MAin trans-uranium (TRU) fuel composition as Np-MOX fuel type. It was loaded into the core region gives significant contribution to reduce the excess reactivity in comparing to mixed oxide (MOX) fuel and in the same time it contributes to increase nuclear fuel breeding capability of the reactor. Neptunium fuel loading scheme in FBR core region gives significant production of Pu-238 as fertile material to absorp neutrons for reducing excess reactivity and additional contribution for fuel breeding.« less

Neutron-induced fission cross section measurements for uranium isotopes 236U and 234U at LANSCE

NASA Astrophysics Data System (ADS)

Laptev, A. B.; Tovesson, F.; Hill, T. S.

2013-04-01

A well established program of neutron-induced fission cross section measurement at Los Alamos Neutron Science Center (LANSCE) is supporting the Fuel Cycle Research program (FC R&D). The incident neutron energy range spans from sub-thermal up to 200 MeV by combining two LANSCE facilities, the Lujan Center and the Weapons Neutron Research facility (WNR). The time-of-flight method is implemented to measure the incident neutron energy. A parallel-plate fission ionization chamber was used as a fission fragment detector. The event rate ratio between the investigated foil and a standard 235U foil is converted into a fission cross section ratio. In addition to previously measured data new measurements include 236U data which is being analyzed, and 234U data acquired in the 2011-2012 LANSCE run cycle. The new data complete the full suite of Uranium isotopes which were investigated with this experimental approach. Obtained data are presented in comparison with existing evaluations and previous data.

Uranium isotope fractionation in biogenic carbonates: biological effects

NASA Astrophysics Data System (ADS)

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

2017-12-01

Recent laboratory experiments have demonstrated small but potentially significant isotope fractionation ( 0.10 ‰ for 238U/235U) during uranium (U) incorporation into abiotic calcite and aragonite, with heavier U isotopes preferentially enriched in the precipitates [1]. In contrast, measurements of natural biogenic carbonates to date have not been able to resolve significant U isotopic fractionation from seawater although this might be expected given a typical measurement precision of ± 0.10 ‰. Determining whether or not biogenic carbonates display U isotope fractionation similar to abiotic carbonates could have important implications for understanding the mechanisms of U incorporation into various biogenic carbonates. Furthermore, because most marine carbonates are biogenic, the extent of isotopic fractionation, if any, could have important implications for the interpretation of sedimentary carbonates record similar to effects observed for Cr and B isotopes [2, 3]. To resolve this discrepancy, we utilized a higher precision 238U/235U method which uses larger sample sizes to improve measurement precision of natural samples to ± 0.02 ‰ (2 se, N = 6) [4]. Using this method, we have surveyed 238U/235U in primary biogenic skeletal carbonates including scleractinian corals, green and red algae, and mollusks, as well as non-skeletal carbonates such as stromatolites, ooids, and carbonate sands from the Bahamas, Gulf of California, and French Polynesia. New high-precision U isotopes measurements reveal that biogenic skeletal carbonates are typically 0.02 - 0.08 ‰ heavier than modern seawater. Scleractinian corals display values closest to seawater (- 0.37 ‰), while green algae, red algae, mollusks, and echinoderms display variable but larger extents of fractionation up to 0.08 ‰. The direction and magnitude of U isotope fractionation in these biogenic precipitates are generally consistent with results from abiotic coprecipitation experiments, but may be subject to variations in U speciation and carbonate chemistry at calcification sites. [1] Chen et a., (2016), GCA, 188, 189-207. [2] Wang et a., (2016), Geobiology, 5, 51-64. [3] Pagani et al., (2005) GCA, 69, 953-961. [4] Andersen et al., (2016) CG, 420, 11-22.

Atmospheric dust contribution to budget of U-series nuclides in weathering profiles. The Mount Cameroon volcano

NASA Astrophysics Data System (ADS)

Pelt, E.; Chabaux, F. J.; Innocent, C.; Ghaleb, B.

2009-12-01

Analysis of U-series nuclides in weathering profiles is developed today for constraining time scale of soil and weathering profile formation (e.g., Chabaux et al., 2008). These studies require the understanding of U-series nuclides sources and fractionation in weathering systems. For most of these studies the impact of aeolian inputs on U-series nuclides in soils is usually neglected. Here, we propose to discuss such an assumption, i.e., to evaluate the impact of dust deposition on U-series nuclides in soils, by working on present and paleo-soils collected on the Mount Cameroon volcano. Recent Sr, Nd, Pb isotopic analyses performed on these samples have indeed documented significant inputs of Saharan dusts in these soils (Dia et al., 2006). We have therefore analyzed 238U-234U-230Th nuclides in the same samples. Comparison of U-Th isotopic data with Sr-Nd-Pb isotopic data indicates a significant impact of the dust input on the U and Th budget of the soils, around 10% for both U and Th. Using Sr-Nd-Pb isotopic data of Saharan dusts given by Dia et al. (2006) we estimate U-Th concentrations and U-Th isotope ratios of dusts compatible with U-Th data obtained on Saharan dusts collected in Barbados (Rydell H.S. and Prospero J.M., 1972). However, the variations of U/Th ratios along the weathering profiles cannot be explained by a simple mixing scenario between material from basalt and from the defined atmospheric dust pool. A secondary uranium migration associated with chemical weathering has affected the weathering profiles. Mass balance calculation suggests that U in soils from Mount Cameroon is affected at the same order of magnitude by both chemical migration and dust accretion. Nevertheless, the Mount Cameroon is a limit case were large dust inputs from continental crust of Sahara contaminate basaltic terrain from Mount Cameroon volcano. Therefore, this study suggests that in other contexts were dust inputs are lower, or the bedrocks more concentrated in U and Th, the dust contribution will not significantly influence U-series dating. Chabaux F., Bourdon B., Riotte J. (2008). U-series Geochemistry in weathering profiles, river waters and lakes. Radioactivity in the Environment, 13, 49-104. Dia A., Chauvel C., Bulourde M. and Gérard M. (2006). Eolian contribution to soils on Mount Cameroon: Isotopic and trace element records. Chem. Geol. 226, 232-252. Rydell H.S. and Prospero J.M. (1972). Uranium and thorium concentrations in wind-borne Saharan dust over the western equatorial north atlantic ocean. EPSL 14, 397-402.

Distinguishing fissions of 232Th, 237Np and 238U with beta-delayed gamma rays

DOE PAGES

Iyengar, A.; Norman, E. B.; Howard, C.; ...

2013-04-08

Measurements of beta-delayed gamma-ray spectra following 14-MeV neutron-induced fissions of 232Th, 238U, and 237Np were conducted at Lawrence Berkeley National Laboratory’s 88-Inch Cyclotron. Spectra were collected for times ranging from 1 minute to 14 hours after irradiation. Lastly, intensity ratios of gamma-ray lines were extracted from the data that allow identification of the fissioning isotope.

Measurement of 238U and 232Th in Petrol, Gas-oil and Lubricant Samples by Using Nuclear Track Detectors and Resulting Radiation Doses to the Skin of Mechanic Workers.

PubMed

Misdaq, M A; Chaouqi, A; Ouguidi, J; Touti, R; Mortassim, A

2015-10-01

Workers in repair shops of vehicles (cars, buses, truck, etc.) clean carburetors, check fuel distribution, and perform oil changes and greasing. To explore the exposure pathway of (238)U and (232)Th and its decay products to the skin of mechanic workers, these radionuclides were measured inside petrol, gas-oil, and lubricant material samples by means of CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs), and corresponding annual committed equivalent doses to skin were determined. The maximum total equivalent effective dose to skin due to the (238)U and (232)Th series from the application of different petrol, gas-oil, and lubricant samples by mechanic workers was found equal to 1.2 mSv y(-1) cm(-2).

U-238 fission and Pu-239 production in subcritical assembly

NASA Astrophysics Data System (ADS)

Grab, Magdalena; Wojciechowski, Andrzej

2018-04-01

The project touches upon an issue of U-238 fission reactions and Pu-239 production reactions in subcritical assembly. The experiment took place in November 2014 at the Dzhelepov Laboratory of Nuclear Problems (JINR, Dubna) using PHASOTRON.Data of this experiment were analyzed in Laboratory of Information Technologies (LIT). Four MCNPX models were considered for simulation: Bertini/Dresnen, Bertini/Abla, INCL4/Drensnen, INCL4/Abla. The main goal of the project was to compare the experimental data and simulation results. We obtain a good agreement of experimental data and computation results especially for detectors placed besides the assembly axis. In addition, the U-238 fission reactions are more probable to be observed in the region of a higher particle energy spectrum, located closer to the assembly axis and the particle beam as well and vice versa Pu-239 production reactions were dominant in the peripheral region of geometry.

Evaluation of potential hazard exposure resulting from DOE waste treatment and disposal at Rollins Environmental Services, Baton Rouge, LA

DOE Office of Scientific and Technical Information (OSTI.GOV)

Not Available

1992-04-01

The equivalent dose rate to populations potentially exposed to wastes shipped to Rollins Environmental Services, Baton Rouge, LA from Oak Ridge and Savannah River Operations of the Department of Energy was estimated. Where definitive information necessary to the estimation of a dose rate was unavailable, bounding assumptions were employed to ensure an overestimate of the actual dose rate experienced by the potentially exposed population. On this basis, it was estimated that a total of about 3.85 million pounds of waste was shipped from these DOE operations to Rollins with a maximum combined total activity of about 0.048 Curies. Populations nearmore » the Rollins site could potentially be exposed to the radionuclides in the DOE wastes via the air pathway after incineration of the DOE wastes or by migration from the soil after landfill disposal. AIRDOS was used to estimate the dose rate after incineration. RESRAD was used to estimate the dose rate after landfill disposal. Calculations were conducted with the estimated radioactive specie distribution in the wastes and, as a test of the sensitivity of the results to the estimated distribution, with the entire activity associated with individual radioactive species such as Cs-137, Ba-137, Sr-90, Co-60, U-234, U-235 and U-238. With a given total activity, the dose rates to nearby individuals were dominated by the uranium species.« less

Reduced probabilities for E2 transitions between excited collective states of triaxial even–even nuclei

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nadyrbekov, M. S., E-mail: nodirbekov@inp.uz; Bozarov, O. A.

Reduced probabilities for intra- and interband E2 transitions in excited collective states of even–even lanthanide and actinide nuclei are analyzed on the basis of a model that admits an arbitrary triaxiality. They are studied in detail in the energy spectra of {sup 154}Sm, {sup 156}Gd, {sup 158}Dy, {sup 162,164}Er, {sup 230,232}Th, and {sup 232,234,236,238}U even–even nuclei. Theoretical and experimental values of the reduced probabilities for the respective E2 transitions are compared. This comparison shows good agreement for all states, including high-spin ones. The ratios of the reduced probabilities for the E2 transitions in question are compared with results following frommore » the Alaga rules. These comparisons make it possible to assess the sensitivity of the probabilities being considered to the presence of quadrupole deformations.« less

Study on radiation production in the charge stripping section of the RISP linear accelerator

NASA Astrophysics Data System (ADS)

Oh, Joo-Hee; Oranj, Leila Mokhtari; Lee, Hee-Seock; Ko, Seung-Kook

2015-02-01

The linear accelerator of the Rare Isotope Science Project (RISP) accelerates 200 MeV/nucleon 238U ions in a multi-charge states. Many kinds of radiations are generated while the primary beam is transported along the beam line. The stripping process using thin carbon foil leads to complicated radiation environments at the 90-degree bending section. The charge distribution of 238U ions after the carbon charge stripper was calculated by using the LISE++ program. The estimates of the radiation environments were carried out by using the well-proved Monte Carlo codes PHITS and FLUKA. The tracks of 238U ions in various charge states were identified using the magnetic field subroutine of the PHITS code. The dose distribution caused by U beam losses for those tracks was obtained over the accelerator tunnel. A modified calculation was applied for tracking the multi-charged U beams because the fundamental idea of PHITS and FLUKA was to transport fully-ionized ion beam. In this study, the beam loss pattern after a stripping section was observed, and the radiation production by heavy ions was studied. Finally, the performance of the PHITS and the FLUKA codes was validated for estimating the radiation production at the stripping section by applying a modified method.

Rapid Radiochemical Method for Isotopic Uranium in Building ...

EPA Pesticide Factsheets

Technical Fact Sheet Analysis Purpose: Qualitative analysis Technique: Alpha spectrometry Method Developed for: Uranium-234, uranium-235, and uranium-238 in concrete and brick samples Method Selected for: SAM lists this method for qualitative analysis of uranium-234, uranium-235, and uranium-238 in concrete or brick building materials. Summary of subject analytical method which will be posted to the SAM website to allow access to the method.

High temperature reaction between sea salt deposit and (U,Zr)O2 simulated corium debris

NASA Astrophysics Data System (ADS)

Takano, Masahide; Nishi, Tsuyoshi

2013-11-01

In order to clarify the possible impacts of seawater injection on the chemical and physical state of the corium debris formed in the severe accident at Fukushima Daiichi Nuclear Power Plants, the high temperature reaction between sea salt deposit and (U,Zr)O2 simulated corium debris (sim-debris) was examined in the temperature range from 1088 to 1668 K. A dense layer of calcium and sodium uranate formed on the surface of a sim-debris pellet at 1275 K under airflow, with the thickness of over 50 μm. When the oxygen partial pressure is low, calcium is likely to dissolve into the cubic sim-debris phase to form solid solution (Ca,U,Zr)O2+x. The diffusion depth was 5-6 μm from the surface, subjected to 1275 K for 12 h. The crystalline MgO remains affixed on the surface as the main residue of salt components. A part of it can also dissolve into the sim-debris.

Concentrations of Radionuclides and Trace Elements in Environmantal Media arond te Dual-Axis Radiographic Hydrodynamic Test Facilit at Los Alamos National Laboratory during 2005

DOE Office of Scientific and Technical Information (OSTI.GOV)

G.J.Gonzales; P.R. Fresquez; C.D.Hathcock

2006-05-15

The Mitigation Action Plan (MAP) for the Dual-Axis Radiographic Hydrodynamic Test (DARHT) facility at Los Alamos National Laboratory requires that samples of biotic and abiotic media be collected after operations began to determine if there are any human health or environmental impacts. The DARHT facility is the Laboratory's principal explosive test facility. To this end, samples of soil and sediment, vegetation, bees, and birds were collected around the facility in 2005 and analyzed for concentrations of {sup 3}H, {sup 137}Cs, {sup 90}Sr, {sup 238}Pu, {sup 239,240}Pu, {sup 241}Am, {sup 234}U, {sup 235}U, {sup 238}U, Ag, As, Ba, Be, Cd, Cr,more » Cu, Hg, Ni, Pb, Sb, Se, and Tl. Bird populations have also been monitored. Contaminant results, which represent up to six sample years since the start of operations, were compared with (1) baseline statistical reference levels (BSRLs) established over a four-year preoperational period before DARHT facility operations, (2) screening levels (SLs), and (3) regulatory standards. Most radionuclides and trace elements were below BSRLs and those few samples that contained radionuclides and trace elements above BSRLs were below SLs. Concentrations of radionuclides and nonradionuclides in biotic and abiotic media around the DARHT facility do not pose a significant human health hazard. The total number of birds captured and number of species represented were similar in 2003 and 2004, but both of these parameters increased substantially in 2005. Periodic interruption of the scope and schedule identified in the MAP generally should have no impact on meeting the intent of the MAP. The risk of not sampling one of the five media in any given year is that if a significant impact to contaminant levels were to occur there would exist a less complete understanding of the extent of the change to the baseline for these media and to the ecosystem as a whole. Since the MAP is a requirement that was established under the regulatory framework of the National Environmental Policy Act, any changes to the monitoring requirements in the MAP must be negotiated with and ultimately approved by the U.S. Department of Energy.« less

The presence of radioactive materials in soil, sand and sediment samples of Potenga sea beach area, Chittagong, Bangladesh: Geological characteristics and environmental implication

NASA Astrophysics Data System (ADS)

Yasmin, Sabina; Barua, Bijoy Sonker; Uddin Khandaker, Mayeen; Kamal, Masud; Abdur Rashid, Md.; Abdul Sani, S. F.; Ahmed, H.; Nikouravan, Bijan; Bradley, D. A.

2018-03-01

Accurate quantification of naturally occurring radioactive materials in soil provides information on geological characteristics, possibility of petroleum and mineral exploration, radiation hazards to the dwelling populace etc. Of practical significance, the earth surface media (soil, sand and sediment) collected from the densely populated coastal area of Chittagong city, Bangladesh were analysed using a high purity germanium γ-ray spectrometer with low background radiation environment. The mean activities of 226Ra (238U), 232Th and 40K in the studied materials show higher values than the respective world average of 33, 36 and 474 Bq/kg reported by the UNSCEAR (2000). The deduced mass concentrations of the primordial radionuclides 238U, 232Th and 40K in the investigated samples are corresponding to the granite rocks, crustal minerals and typical rocks respectively. The estimated mean value of 232Th/238U for soil (3.98) and sediment (3.94) are in-line with the continental crustal average concentration of 3.82 for typical rock range reported by the National Council on Radiation Protection and Measurements (NCRP). But the tonalites and more silicic rocks elevate the mean value of 232Th/238U for sand samples amounting to 4.69. This indicates a significant fractionation during weathering or associated with the metasomatic activity in the investigated area of sand collection.

Evidence of isotopic fractionation of natural uranium in cultured human cells

NASA Astrophysics Data System (ADS)

Paredes, Eduardo; Avazeri, Emilie; Malard, Véronique; Vidaud, Claude; Reiller, Pascal E.; Ortega, Richard; Nonell, Anthony; Isnard, Hélène; Chartier, Frédéric; Bresson, Carole

2016-12-01

The study of the isotopic fractionation of endogen elements and toxic heavy metals in living organisms for biomedical applications, and for metabolic and toxicological studies, is a cutting-edge research topic. This paper shows that human neuroblastoma cells incorporated small amounts of uranium (U) after exposure to 10 µM natural U, with preferential uptake of the 235U isotope with regard to 238U. Efforts were made to develop and then validate a procedure for highly accurate n(238U)/n(235U) determinations in microsamples of cells. We found that intracellular U is enriched in 235U by 0.38 ± 0.13‰ (2σ, n = 7) relative to the exposure solutions. These in vitro experiments provide clues for the identification of biological processes responsible for uranium isotopic fractionation and link them to potential U incorporation pathways into neuronal cells. Suggested incorporation processes are a kinetically controlled process, such as facilitated transmembrane diffusion, and the uptake through a high-affinity uranium transport protein involving the modification of the uranyl (UO22+) coordination sphere. These findings open perspectives on the use of isotopic fractionation of metals in cellular models, offering a probe to track uptake/transport pathways and to help decipher associated cellular metabolic processes.

Evidence of isotopic fractionation of natural uranium in cultured human cells

PubMed Central

Paredes, Eduardo; Avazeri, Emilie; Malard, Véronique; Vidaud, Claude; Reiller, Pascal E.; Ortega, Richard; Nonell, Anthony; Isnard, Hélène; Chartier, Frédéric; Bresson, Carole

2016-01-01

The study of the isotopic fractionation of endogen elements and toxic heavy metals in living organisms for biomedical applications, and for metabolic and toxicological studies, is a cutting-edge research topic. This paper shows that human neuroblastoma cells incorporated small amounts of uranium (U) after exposure to 10 µM natural U, with preferential uptake of the 235U isotope with regard to 238U. Efforts were made to develop and then validate a procedure for highly accurate n(238U)/n(235U) determinations in microsamples of cells. We found that intracellular U is enriched in 235U by 0.38 ± 0.13‰ (2σ, n = 7) relative to the exposure solutions. These in vitro experiments provide clues for the identification of biological processes responsible for uranium isotopic fractionation and link them to potential U incorporation pathways into neuronal cells. Suggested incorporation processes are a kinetically controlled process, such as facilitated transmembrane diffusion, and the uptake through a high-affinity uranium transport protein involving the modification of the uranyl (UO22+) coordination sphere. These findings open perspectives on the use of isotopic fractionation of metals in cellular models, offering a probe to track uptake/transport pathways and to help decipher associated cellular metabolic processes. PMID:27872304

Evidence of isotopic fractionation of natural uranium in cultured human cells.

PubMed

Paredes, Eduardo; Avazeri, Emilie; Malard, Véronique; Vidaud, Claude; Reiller, Pascal E; Ortega, Richard; Nonell, Anthony; Isnard, Hélène; Chartier, Frédéric; Bresson, Carole

2016-12-06

The study of the isotopic fractionation of endogen elements and toxic heavy metals in living organisms for biomedical applications, and for metabolic and toxicological studies, is a cutting-edge research topic. This paper shows that human neuroblastoma cells incorporated small amounts of uranium (U) after exposure to 10 µM natural U, with preferential uptake of the 235 U isotope with regard to 238 U. Efforts were made to develop and then validate a procedure for highly accurate n( 238 U)/n( 235 U) determinations in microsamples of cells. We found that intracellular U is enriched in 235 U by 0.38 ± 0.13‰ (2σ, n = 7) relative to the exposure solutions. These in vitro experiments provide clues for the identification of biological processes responsible for uranium isotopic fractionation and link them to potential U incorporation pathways into neuronal cells. Suggested incorporation processes are a kinetically controlled process, such as facilitated transmembrane diffusion, and the uptake through a high-affinity uranium transport protein involving the modification of the uranyl (UO 2 2+ ) coordination sphere. These findings open perspectives on the use of isotopic fractionation of metals in cellular models, offering a probe to track uptake/transport pathways and to help decipher associated cellular metabolic processes.

Bioaccumulation of the artificial Cs-137 and the natural radionuclides Th-234, Ra-226, and K-40 in the fruit bodies of Basidiomycetes in Greece.

PubMed

Kioupi, Vasiliki; Florou, Heleny; Kapsanaki-Gotsi, Evangelia; Gonou-Zagou, Zacharoula

2016-01-01

The bioaccumulation of artificial Cs-137 and natural radionuclides Th-234, Ra-226, and K-40 by Basidiomycetes of several species is studied and evaluated in relation to their substratum soils. For this reason, 32 fungal samples, representing 30 species of Basidiomycetes, were collected along with their substratum soil samples, from six selected sampling areas in Greece. The fungal fruit bodies and the soil samples were properly treated and the activity concentrations of the studied radionuclides were measured by gamma spectroscopy. The measured radioactivity levels ranged as follows: Cs-137 from <0.1 to 87.2 ± 0.4 Bq kg(-1) fresh weight (F.W.), Th-234 from <0.5 ± 0.9 to 28.3 ± 25.5 Bq kg(-1) F.W., Ra-226 from <0.3 to 1.0 ± 0.5 Bq kg(-1) F.W., and K-40 from 56.4 ± 3.0 to 759.0 ± 28.3 Bq kg(-1) F.W. The analysis of the results supported that the bioaccumulation of the studied natural radionuclides and Cs-137 is dependent on the species and the functional group of the fungi. Fungi were found to accumulate Th-234 and not U-238. What is more, potential bioindicators for each radionuclide among the 32 species studied could be suggested for each habitat, based on their estimated concentration ratios (CRs). The calculation of the CRs' mean values for each radionuclide revealed a rank in decreasing order for all the species studied.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arbanas, G; Dietrich, F S; Kerman, A K

A method for computing direct-semidirect (DSD) neutron radiative capture is presented and applied to thermal neutron capture on {sup 19}F, {sup 27}Al, {sup 28,29.30}Si, {sup 35,37}Cl, {sup 39,41}K, {sup 56}Fe, and {sup 238}U, in support of data evaluation effort at the O.R.N.L. The DSD method includes both direct and semidirect capture; the latter is a core-polarization term in which the giant dipole resonance is formed. We study the effects of a commonly used ''density'' approximation to the EM operator and find it to be unsatisfactory for the nuclei considered here. We also study the magnitude of semidirect capture relative tomore » the pure direct capture. Furthermore, we compare our results with those obtained from another direct capture code (Tedca [17]). We also compare our results with those obtained from analytical expression for external capture derived by Lane and Lynn [3], and its extension to include internal capture [7]. To estimate the effect of nuclear deformation on direct capture, we computed direct thermal capture on {sup 238}U with and without imposition of spherical symmetry. Direct capture for a spherically symmetric {sup 238}U was approximately 6 mb, while a quadrupole deformation of 0.215 on the shape of {sup 238}U lowers this cross section down to approximately 2 mb. This result suggests that effects of nuclear deformation on direct capture warrant a further study. We also find out that contribution to the direct capture on {sup 238}U from the nuclear interior significantly cancels that coming from the exterior region, and hence both contributions must be taken into account. We reproduced a well known discrepancy between the computed and observed branching ratios in {sup 56}Fe(n,{gamma}). This will lead us to revisit the concept of doorway states in the particle-hole model.« less

Gamma-spectrometric measurement of radioactivity in agricultural soils of the Lombardia region, northern Italy.

PubMed

Guidotti, Laura; Carini, Franca; Rossi, Riccardo; Gatti, Marina; Cenci, Roberto M; Beone, Gian Maria

2015-04-01

This work is part of a wider monitoring project of the agricultural soils in Lombardia, which aims to build a database of topsoil properties and the potentially toxic elements, organic pollutants and gamma emitting radionuclides that the topsoils contain. A total of 156 agricultural soils were sampled according to the LUCAS (Land Use/Cover Area frame statistical Survey) standard procedure. The aim was to provide a baseline to document the conditions present at the time of sampling. The results of the project concerning soil radioactivity are presented here. The aim was to assess the content of (238)U, (232)Th, (137)Cs and (40)K by measuring soil samples by gamma spectrometry. (238)U, (232)Th and (40)K activities range 24-231, 20-70, and 242-1434 Bq kg(-1) respectively. The geographic distribution of (238)U reflects the geophysical framework of the Lombardia region: the soils with high content of uranium are distributed for the most part in the South Alpine belt, where the presence of magmatic rocks is widespread. These soils show an higher activity of (238)U than of (232)Th. The (238)U activities become lower than (232)Th when soils are located in the plain, originating from basic sedimentary rocks. (137)Cs activity ranges 0.4-86.8 kBq m(-2). The lowest activity of (137)Cs is in the plain, whereas the highest is in the North on soils kept as lawn or pasture. The (137)Cs activity of some samples suggests the presence of accumulation processes that lead to (137)Cs enriched soils. This is the first survey of gamma emitting radionuclides in Lombardia that is based on the LUCAS standard sampling. The results from this monitoring campaign are important for the human radiation exposure and provide the zero point, which will be useful for assessing future effects due to external factors such as human activities. Copyright © 2015 The Authors. Published by Elsevier Ltd.. All rights reserved.

Constraining the redox landscape of the mid-Proterozoic oceans: new insights from the carbonate uranium isotope record

NASA Astrophysics Data System (ADS)

Gilleaudeau, G. J.; Kaufman, A. J.; Luo, G.; Romaniello, S. J.; Zhang, F.; Kah, L. C.; Azmy, K.; Bartley, J. K.; Sahoo, S. K.; Knoll, A. H.; Anbar, A. D.

2017-12-01

The redox landscape of the global oceans during the prolonged period between the Great Oxidation Event (GOE) and the Neoproterozoic Oxygenation Event (NOE) is a topic of considerable debate. Data from local redox proxies such as iron speciation suggest largely ferruginous conditions in the subsurface oceans (with the exception of one report of oxic subsurface waters) and a variable degree of euxinia in shallow shelf and epeiric sea environments. There is general consensus that anoxia was more widespread than in the modern ocean, but quantifying the degree of seafloor anoxia is challenging given that most redox proxies are inherently local and/or based on the relatively sparse black shale record. Here, we present new uranium (U) isotope data from carbonate rocks than span the mid-Proterozoic Eon. U-isotopes operate as a proxy for seafloor anoxia because the δ238U value of seawater is largely controlled by the size of the anoxic/euxinic U sink, which preferentially removes isotopically heavy 238U, leaving the oceans enriched in 235U. Our compilation of data from mid-Proterozoic successions reveals δ238U values similar to modern seawater (-0.39 ± 0.19 ‰ [1 s.d.] for the Gaoyuzhuang, Angmaat, El Mreiti, Vazante, and Turukhansk successions spanning 1.5 to 0.9 Ga). Given the potential for an isotopic offset between carbonate minerals and seawater of up to 0.3 ‰, we suggest that mid-Proterozoic seawater had a δ238U value generally between -0.4 and -0.7 ‰, which is lower than modern seawater, but higher than has been inferred for intervals of expanded anoxia elsewhere in Earth history. These results are consistent with recently published U-isotope data from the 1.36 Ga Velkerri Formation, and suggest that large portions of the seafloor may have been covered by at least weakly oxygenated waters during the mid-Proterozoic Eon. Uncertainty remains, however, because the isotopic effects of the non-euxinic anoxic sink are poorly constrained. Nonetheless, our data suggest that euxinia was spatially restricted and that suboxic to oxic conditions may have been more widespread than previously thought. Future work should seek to reconcile possible interpretations of our data with recent pO2 estimates to provide a more holistic view of mid-Proterozoic redox conditions.

The Typical Number of Antiprotons Necessary to Heat the Hot Spot in the D-T Fuel Doped with U

NASA Astrophysics Data System (ADS)

Shmatov, M. L.

Fast ignition scenario with heating the hot spot by products of annihilation of antiprotons in the D-T fuel doped with U238 is considered. It is shown that in this scenario the hot spot is being heated effectively only by the fission fragments arising due to annihilation of the antiprotons on the nuclei of uranium. The presented model predicts that fast ignition can be provided by injection of (1.3 to 4.4) x 1015 antiprotons into the D-T fuel compressed to the density of about 200 g/cm3 and containing one nucleus of U238 per about one thousand nuclei of hydrogen isotopes.

Sharpening the U-Th Chronometer: Progress and Outlook

NASA Astrophysics Data System (ADS)

McLean, N. M.; Condon, D. J.; Henderson, G. M.; Richards, D. A.; Noble, S.; Mason, A.

2013-12-01

Uranium is incorporated into a variety of natural materials when they form, including carbonates like speleothems and corals. The two most abundant naturally occurring uranium isotopes, 238U and 235U, decay to 206Pb and 207Pb over long timescales with half-lives of 4.5 and 0.7 billion years respectively, but transition through several intermediate daughter isotopes with shorter half-lives first. Fractionation between these daughter isotopes, including 234U, 230Th, and 231Pa, and their parent isotopes, followed by their time-dependent return to secular equilibrium over the course of up to ~800 kyr, forms the basis for U-series geochronology, and allows speleothems and corals to be precisely dated. These carbonates often additionally incorporate chemical and isotopic signatures (e.g., trace elements, δ18O and δ13C) from the environment in which they form, and thus are some of the best dated paleoclimate archives, offering clues about past and future conditions for life on Earth. Over the past decade, the analytical precision of U-series isotope measurements has improved dramatically, largely due to the steadily increasing sensitivity of multiple-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Analytical uncertainties in U-Th dates now approach or are better than 0.1% (2σ), for instance ×100 years for a speleothem or coral that is 130 kyr old (Cheng et al., 2013). However, the accuracy of U-series dates also depends on the accuracy of tracer calibrations, reference solutions and data reduction protocols, which has not kept pace in many laboratories. This means that dates measured in different labs, while impressively precise, may not be directly comparable. To address issues of inter-laboratory bias and improve the accuracy and inter-comparability of U-Th dates, we have instigated work in three related directions. First, we report on the mixing of three synthetic U-Th age solutions, created by combining high-purity mono-isotopic solutions to mimic the isotopic composition of commonly analyzed materials. These age solutions will form the basis for an inter-laboratory comparison and serve as international reference materials for assessing long-term reproducibility. Second is the creation of several U-Th gravimetric solutions, which can be used to calibrate the mixed 229Th-236U×233U tracers used in the community without having to rely on materials assumed to be in secular equilibrium. Tracers calibrated against these solutions, and therefore U-Th dates measured with these tracers, will be fully metrologically traceable. Finally, we report progress on and important considerations in developing data reduction and uncertainty propagation protocols for calculating U-Th dates and constructing and interpreting U-Th age models. Reference: Cheng et al. (2013) EPSL 371-372, 82-91

Void reactivity feedback analysis for U-based and Th-based LWR incineration cycles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lindley, B.A.; Parks, G.T.; Franceschini, F.

2013-07-01

In reduced-moderation LWRs, an external supply of transuranic (TRU) can be incinerated by mixing it with a fertile isotope ({sup 238}U or {sup 232}Th) and recycling all the actinides after each cycle. Performance is limited by coolant reactivity feedback - the moderator density coefficient (MDC) must be kept negative. The MDC is worse when more TRU is loaded, but TRU feed is also needed to maintain criticality. To assess the performance of this fuel cycle in different neutron spectra, three LWRs are considered: 'reference' PWRs and reduced-moderation PWRs and BWRs. The MDC of the equilibrium cycle is analysed by reactivitymore » decomposition with perturbed coolant density by isotope and neutron energy. The results show that using {sup 232}Th as a fertile isotope yields superior performance to {sup 238}U. This is due essentially to the high resonance η of U bred from Th (U3), which increases the fissility of the U3-TRU isotope vector in the Th-fueled system relative to the U-fueled system, and also improves the MDC in a sufficiently hard spectrum. Spatial separation of TRU and U3 in the Th-fueled system renders further improvement by hardening the neutron spectrum in the TRU and softening it in the U3. This improves the TRU η and increases the negative MDC contribution from reduced thermal fission in U3. (authors)« less

Improved spatial resolution for U-series dating of opal at Yucca Mountain, Nevada, USA, using ion-microprobe and microdigestion methods

USGS Publications Warehouse

Paces, J.B.; Neymark, L.A.; Wooden, J.L.; Persing, H.M.

2004-01-01

Two novel methods of in situ isotope analysis, ion microprobe and microdigestion, were used for 230Th/U and 234U/238U dating of finely laminated opal hemispheres formed in unsaturated felsic tuff at Yucca Mountain, Nevada, proposed site for a high-level radioactive waste repository. Both methods allow analysis of layers as many as several orders of magnitude thinner than standard methods using total hemisphere digestion that were reported previously. Average growth rates calculated from data at this improved spatial resolution verified that opal grew at extremely slow rates over the last million years. Growth rates of 0.58 and 0.69 mm/m.y. were obtained for the outer 305 and 740 ??m of two opal hemispheres analyzed by ion microprobe, and 0.68 mm/m.y. for the outer 22 ??m of one of these same hemispheres analyzed by sequential microdigestion. These Pleistocene growth rates are 2 to 10 times slower than those calculated for older secondary calcite and silica mineral coatings deposited over the last 5 to 10 m.y. dated by the U-Pb method and may reflect differences between Miocene and Pleistocene seepage flux. The microdigestion data also imply that opal growth rates may have varied over the last 40 k.y. These data are the first indication that growth rates and associated seepage in the proposed repository horizon may correlate with changes in late Pleistocene climate, involving faster growth during wetter, cooler climates (glacial maximum), slower growth during transition climates, and no growth during the most arid climate (modern). Data collected at this refined spatial scale may lead to a better understanding of the hydrologic variability expected within the thick unsaturated zone at Yucca Mountain over the time scale of interest for radioactive waste isolation. ?? 2004 Elsevier Ltd.

Natural radionuclides in fish species from surface water of Bagjata and Banduhurang uranium mining areas, East Singhbhum, Jharkhand, India.

PubMed

Giri, Soma; Singh, Gurdeep; Jha, V N; Tripathi, R M

2010-11-01

To study the natural radionuclides in the freshwater fish samples around the uranium mining areas of Bagjata and Banduhurang, East Singhbhum, Jharkhand, India. The naturally occurring radioisotopes of uranium, U(nat), consisting of (234)U, (235)U and (238)U; (226)Ra, (230)Th and (210)Po were analysed in the fish samples from the surface water of Bagjata and Banduhurang mining areas after acid digestion. The ingestion dose, concentration factor and excess lifetime cancer risk of the radionuclides were estimated. The geometric mean activity of U(nat), (226)Ra, (230)Th and (210)Po in the fish samples was found to be 0.05, 0.19, 0.29 and 0.95 Bq kg(-1)(fresh) (Becquerel per kilogram fresh fish), respectively, in the Bagjata mining area, while for Banduhurang mining area it was estimated to be 0.08, 0.41, 0.22 and 2.48 Bq kg(-1)(fresh), respectively. The ingestion dose was computed to be 1.88 and 4.16 μSvY(-1), respectively, for both the areas which is much below the 1 mSv limit set in the new International Commission on Radiological Protection (ICRP) recommendations. The estimation of the Concentration Factors (CF) reveal that the CF from water is greater than 1 l/kg(-1)in most of the cases while from sediment CF is less than 1. The excess individual lifetime cancer risk due to the consumption of fish was calculated to be 2.53 × 10(-5) and 6.48 × 10(-5), respectively, for Bagjata and Banduhurang areas, which is within the acceptable excess individual lifetime cancer risk value of 1 × 10(-4). The study confirms that current levels of radioactivity do not pose a significant radiological risk to freshwater fish consumers.

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.

Structure and migration in U.S. Blumeria graminis f. sp. tritici populations

USDA-ARS?s Scientific Manuscript database

While wheat powdery mildew occurs throughout the south-central and eastern U.S.A, epidemics are especially damaging in the Mid-Atlantic states. The structure of the U.S. Blumeria graminis f. sp. tritici population was assessed based on a sample of 238 single-spored isolates. The isolates were coll...

46 CFR 282.22 - Maintenance (upkeep) and repairs.

Code of Federal Regulations, 2010 CFR

2010-10-01

...) (Percent) Japan Japan 85 36.21 30.78 U.S 15 0 0 100 30.78 23.4 7.20 Norway Norway 15 44.72 6.71 Netherlands 20 43.23 8.65 Japan 45 36.21 16.29 U.S 20 0 0 100 31.65 31.1 9.84 United Kingdom U.K 80 19.00 15.20...

Systematic investigation of cluster radioactivity for uranium isotopes

NASA Astrophysics Data System (ADS)

Seif, W. M.; Amer, Laila H.

2018-01-01

The most probable cluster decays that can be observed for 217-238U isotopes are investigated. We identified the more-probable decays that commonly manifest themselves via cold valleys in the driving potentials with respect to the mass number and the atomic number, individually. The calculations are performed using the Skyrme-SLy4 nucleon-nucleon interaction, within the frame work of the performed cluster model. Among the indicated favored decays that involve emitted light clusters heavier than α-particle, twenty six decay modes display calculated half-life less than 1022 years, with branching ratio larger than 10-14%. The estimated branching ratio for the α-decay of 237U, that did not observed yet, is B = 2.1 ×10-10% (Tα = 8.7 ×109 years). The indicated most probable decays that did not observed yet include the 22Ne decay of 232U, 25Ne and 32Si decays of 233U, 24Ne and 29Mg decays of 235U, and the 34Si and 30Mg decay modes of 238U, with 10-14 < B(%) <10-7.

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/235U. GCA 72,345-359 [2] Wang X. et al. (2015) Isotope fractionation during oxidation of tetravalent uranium by dissolved oxygen. GCA 150, 160-170

236U measurement with accelerator mass spectrometry at CIAE

NASA Astrophysics Data System (ADS)

Wang, Xianggao; Jiang, Shan; He, Ming; Dong, Kejun; Wang, Wei; Li, Chaoli; He, Guozhu; Li, Shizhuo; Gong, Jie; Lu, Liyuan; Wu, Shaoyong

2010-07-01

236U is a long-lived radioactive isotope which is produced principally by thermal neutron capture on 235U. 236U may be potentially applied in geological research and nuclear safeguards. Accelerator mass spectrometry is presently the most sensitive technique for the measurement of 236U and a measurement method for long-lived heavy ion 236U has been developed. The set-up uses a dedicated injector and the newly proposed 208Pb 16O2- molecular ions for the simulation of 236U ion transport. A sensitivity of lower than 10 -10 has been achieved for the isotopic ratio 236U/ 238U in present work.

238U Mössbauer study on the magnetic properties of uranium-based heavy fermion superconductors

NASA Astrophysics Data System (ADS)

Tsutsui, Satoshi; Nakada, Masami; Nasu, Saburo; Haga, Yoshinori; Honma, Tetsuo; Yamamoto, Etsuji; Ohkuni, Hitoshi; Ōnuki, Yoshichika

2000-07-01

We have performed 238U Mössbauer spectroscopy of uranium-based heavy fermion superconductors, UPd2Al3 and URu2Si2, in order to investigate their physical properties, mainly their magnetic properties. The slow relaxation of magnetic hyperfine interaction in a paramagnetic state and the static hyperfine field has been observed in an antiferromagnetic ordered state for each compound. The line-widths have maximum at their characteristic temperatures where their magnetic susceptibilities have maximum values.

Natural and artificial radionuclides in the Suez Canal bottom sediments and stream water

NASA Astrophysics Data System (ADS)

El-Tahawy, M. S.; Farouk, M. A.; Ibrahiem, N. M.; El-Mongey, S. A. M.

1994-07-01

Concentration of natural and artificial radionuclides in Suez Canal bottom sediments and stream water have been measured using γ spectrometers based on a hyper-pure Ge detector. The activity concentrations of 238U series, 232Th series and 40K did not exceed 16.0, 15.5 and 500.0 Bq kg-1 dry weight for sediments. The activity concentration of 238U series and 40K did not exceed 0.6 and 18.0 Bq 1-1 for stream water.

230Th-234U Model-Ages of Some Uranium Standard Reference Materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Williams, R W; Gaffney, A M; Kristo, M J

The 'age' of a sample of uranium is an important aspect of a nuclear forensic investigation and of the attribution of the material to its source. To the extent that the sample obeys the standard rules of radiochronometry, then the production ages of even very recent material can be determined using the {sup 230}Th-{sup 234}U chronometer. These standard rules may be summarized as (a) the daughter/parent ratio at time=zero must be known, and (b) there has been no daughter/parent fractionation since production. For most samples of uranium, the 'ages' determined using this chronometer are semantically 'model-ages' because (a) some assumptionmore » of the initial {sup 230}Th content in the sample is required and (b) closed-system behavior is assumed. The uranium standard reference materials originally prepared and distributed by the former US National Bureau of Standards and now distributed by New Brunswick Laboratory as certified reference materials (NBS SRM = NBL CRM) are good candidates for samples where both rules are met. The U isotopic standards have known purification and production dates, and closed-system behavior in the solid form (U{sub 3}O{sub 8}) may be assumed with confidence. We present here {sup 230}Th-{sup 234}U model-ages for several of these standards, determined by isotope dilution mass spectrometry using a multicollector ICP-MS, and compare these ages with their known production history.« less

Morphological and compositional study of 238U thin film targets for nuclear experiments

NASA Astrophysics Data System (ADS)

Sibbens, Goedele; Ernstberger, Markus; Gouder, Thomas; Marouli, Maria; Moens, André; Seibert, Alice; Vanleeuw, David; Zúñiga, Martin Vargas; Wiss, Thierry; Zampella, Mariavittoria; Zuleger, Evelyn

2018-05-01

The uncertainty in neutron cross section values strongly depends on the quality and characteristics of the deposited actinide films which are used as "targets" in the nuclear experiments. Until recently, at the Joint Research Centre in Geel (JRC-Geel), mass and areal densities of actinide layers were determined by measuring activity (using alpha-particle counting), isotopic composition (using thermal ionisation mass spectrometry) and diameter. In this study a series of 238U deposits, prepared by molecular plating and vacuum deposition on different substrates, were characterized with additional non-destructive and destructive analysis techniques. The quality of the deposits was investigated by autoradiography, high-resolution alpha-particle spectrometry, and scanning electron microscopy. The elemental composition was determined by x-ray photoelectron spectroscopy and inductively coupled plasma mass spectrometry. The latter technique was also applied on the U3O8 starting material and the converted UF4 powder. This paper compares the quality and morphology of deposited 238U films prepared by molecular plating and vacuum deposition on various backings, including their elemental composition determined by different characterization techniques. Also discussed are problems in target preparation and characterization.

Study of hot thermally fissile nuclei using relativistic mean field theory

NASA Astrophysics Data System (ADS)

Quddus, Abdul; Naik, K. C.; Patra, S. K.

2018-07-01

We have studied the properties of hot 234,236U and 240Pu nuclei in the framework of relativistic mean field formalism. The recently developed FSUGarnet and IOPB-I parameter sets are implemented for the first time to deform nuclei at finite temperature. The results are compared with the well known NL3 set. The said isotopes are structurally important because of the thermally fissile nature of 233,235U and 239Pu as these nuclei (234,236U and 240Pu) are formed after the absorption of a thermal neutron, which undergoes fission. Here, we have evaluated the nuclear properties, such as shell correction energy, neutron-skin thickness, quadrupole and hexadecapole deformation parameters and asymmetry energy coefficient for these nuclei as a function of temperature.

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)

RAPID DETERMINATION OF ACTINIDES IN URINE BY INDUCTIVELY-COUPLED PLASMA MASS SPECTROMETRY AND ALPHA SPECTROMETRY: A HYBRID APPROACH

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maxwell, S.; Jones, V.

2009-05-27

A new rapid separation method that allows separation and preconcentration of actinides in urine samples was developed for the measurement of longer lived actinides by inductively coupled plasma mass spectrometry (ICP-MS) and short-lived actinides by alpha spectrometry; a hybrid approach. This method uses stacked extraction chromatography cartridges and vacuum box technology to facilitate rapid separations. Preconcentration, if required, is performed using a streamlined calcium phosphate precipitation. Similar technology has been applied to separate actinides prior to measurement by alpha spectrometry, but this new method has been developed with elution reagents now compatible with ICP-MS as well. Purified solutions are splitmore » between ICP-MS and alpha spectrometry so that long- and short-lived actinide isotopes can be measured successfully. The method allows for simultaneous extraction of 24 samples (including QC samples) in less than 3 h. Simultaneous sample preparation can offer significant time savings over sequential sample preparation. For example, sequential sample preparation of 24 samples taking just 15 min each requires 6 h to complete. The simplicity and speed of this new method makes it attractive for radiological emergency response. If preconcentration is applied, the method is applicable to larger sample aliquots for occupational exposures as well. The chemical recoveries are typically greater than 90%, in contrast to other reported methods using flow injection separation techniques for urine samples where plutonium yields were 70-80%. This method allows measurement of both long-lived and short-lived actinide isotopes. 239Pu, 242Pu, 237Np, 243Am, 234U, 235U and 238U were measured by ICP-MS, while 236Pu, 238Pu, 239Pu, 241Am, 243Am and 244Cm were measured by alpha spectrometry. The method can also be adapted so that the separation of uranium isotopes for assay is not required, if uranium assay by direct dilution of the urine sample is preferred instead. Multiple vacuum box locations may be set-up to supply several ICP-MS units with purified sample fractions such that a high sample throughput may be achieved, while still allowing for rapid measurement of short-lived actinides by alpha spectrometry.« less

Episodic Holocene eruption of the Salton Buttes rhyolites, California, from paleomagnetic, U-Th, and Ar/Ar dating

USGS Publications Warehouse

Wright, Heather M.; Vazquez, Jorge A.; Champion, Duane E.; Calvert, Andrew T.; Mangan, Margaret T.; Stelten, Mark E.; Cooper, Kari M.; Herzig, Charles; Schriener Jr., Alexander

2015-01-01

In the Salton Trough, CA, five rhyolite domes form the Salton Buttes: Mullet Island, Obsidian Butte, Rock Hill, North and South Red Hill, from oldest to youngest. Results presented here include 40Ar/39Ar anorthoclase ages, 238U-230Th zircon crystallization ages, and comparison of remanent paleomagnetic directions with the secular variation curve, which indicate that all domes are Holocene. 238U-230Th zircon crystallization ages are more precise than but within uncertainty of 40Ar/39Ar anorthoclase ages, suggesting that zircon crystallization proceeded until shortly before eruption in all cases except one. Remanent paleomagnetic directions require three eruption periods: (1) Mullet Island, (2) Obsidian Butte, and (3) Rock Hill, North Red Hill, and South Red Hill. Borehole cuttings logs document up to two shallow tephra layers. North and South Red Hills likely erupted within 100 years of each other, with a combined 238U-230Th zircon isochron age of: 2.83 ± 0.60 ka (2 sigma); paleomagnetic evidence suggests this age predates eruption by hundreds of years (1800 cal BP). Rock Hill erupted closely in time to these eruptions. The Obsidian Butte 238U-230Th isochron age (2.86 ± 0.96 ka) is nearly identical to the combined Red Hill age, but its Virtual Geomagnetic Pole position suggests a slightly older age. The age of aphyric Mullet Island dome is the least well constrained: zircon crystals are resorbed and the paleomagnetic direction is most distinct; possible Mullet Island ages include ca. 2300, 5900, 6900, and 7700 cal BP. Our results constrain the duration of Salton Buttes volcanism to between ca. 5900 and 500 years.

Results of The Excreta Bioassay Quality Control Program For April 1, 2010 Through March 31, 2011

DOE Office of Scientific and Technical Information (OSTI.GOV)

Antonio, Cheryl L.

2012-07-19

A total of 76 urine samples and 10 spiked fecal samples were submitted during the report period (April 1, 2010 through March 31, 2011) to GEL Laboratories, LLC in South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for 14C, Sr, for 238Pu, 239Pu, 241Am, 243Am, 235U, 238U, 238U-mass and fecal analyses for 241Am, 238Pu and 239Pu were tested this year. The number of QC urine samples submitted during the report period represented 1.1% of the total samples submitted. In addition to the samples provided by IDP,more » GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 31% of the analyses processed by GEL during the first year of contract 112512 were quality control samples. GEL tested the performance of 23 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty except the slightly elevated relative bias for 243,244Cm (Table 4).« less

Validation of the U-238 inelastic scattering neutron cross section through the EXCALIBUR dedicated experiment

NASA Astrophysics Data System (ADS)

Leconte, Pierre; Bernard, David

2017-09-01

EXCALIBUR is an integral transmission experiment based on the fast neutron source produced by the bare highly enriched fast burst reactor CALIBAN, located in CEA/DAM Valduc (France). Two experimental campaigns have been performed, one using a sphere of diameter 17 cm and one using two cylinders of 17 cm diameter 9 cm height, both made of metallic Uranium 238. A set of 15 different dosimeters with specific threshold energies have been employed to provide information on the neutron flux attenuation as a function of incident energy. Measurements uncertainties are typically in the range of 0.5-3% (1σ). The analysis of these experiments is performed with the TRIPOLI4 continuous energy Monte Carlo code. A calculation benchmark with validated simplifications is defined in order to improve the statistical convergence under 2%. Various 238U evaluations have been tested: JEFF-3.1.1, ENDF/B-VII.1 and the IB36 evaluation from IAEA. A sensitivity analysis is presented to identify the contribution of each reaction cross section to the integral transmission rate. This feedback may be of interest for the international effort on 238U, through the CIELO project.

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 non-fractionating oxidation, is occurring within this zone. Thus, release of uranium from the NRZs may play a critical role in the persistence of groundwater contamination at these sites.

Distinguishing Fissile From Non-Fissile Materials Using Linearly Polarized Gamma Rays

NASA Astrophysics Data System (ADS)

Mueller, J. M.; Ahmed, M. W.; Karwowski, H. J.; Myers, L. S.; Sikora, M. H.; Weller, H. R.; Zimmerman, W. R.; Randrup, J.; Vogt, R.

2014-03-01

Photofission of 232Th, 233 , 235 , 238U, 237Np, and 239,240Pu was induced by nearly 100% linearly polarized, high intensity (~107 γs per second), and nearly-monoenergetic γ-ray beams of energies between 5.3 and 7.6 MeV at the High Intensity γ-ray Source (HI γS). An array of 12-18 liquid scintillating detectors was used to measure prompt fission neutron yields. The ratio of prompt fission neutron yields parallel to the plane of beam polarization to the yields perpendicular to this plane was measured as a function of beam and neutron energy. A ratio near unity was found for 233,235U, 237Np, and 239Pu while a significant ratio (~1.5-3) was found for 232Th, 238U, and 240Pu. This large difference could be used to distinguish fissile isotopes (such as 233,235U and 239Pu) from non-fissile isotopes (such as 232Th, 238U, and 240Pu). The measured ratios agree with the results of a fission calculation (FREYA) which used with previously measured photofission fragment angular distributions as input. Partially supported by DHS (2010-DN-077-ARI046-02), DOE (DE-AC52-07NA27344 and DE-AC02-05CH11231), and the DOE Office of Science Graduate Fellowship Program (DOE SCGF).

Dynamics of melt generation beneath mid-ocean ridge axes: Theoretical analysis based on 238- 230Th- 226Ra and 235U- 231Pa disequilibria

NASA Astrophysics Data System (ADS)

Qin, Zhenwei

1993-04-01

Although slow melting favors the generation of basaltic melt from a mantle matrix with large radioactive disequilibrium between two actinide nuclides ( MCKENZIE, 1985a), it results in long residence time in a magma chamber, during which the disequilibrium may be removed. An equilibrium melting model modified after MCKENZIE (1985a) is presented here which suggests that, for a given actinide parent-daughter pair, there exists a specific melting rate at which disequilibrium between these two nuclides reaches its maximum. This melting rate depends on the decay constant of the daughter nuclide concerned and the magma chamber volume scaled to that of its source. For a given scaled chamber size, large radioactive disequilibrium between two actinide nuclides in basalts will be observed if the melting rate is such that the residence time of the magma in the chamber is comparable to the mean life of the daughter nuclide. With a chamber size 1% in volume of the melting source, the melting rates at which maximum disequilibrium in basalts is obtained are 10 -7, 2 × 10 -7 and 3 × 10 -6y-1, respectively, for 238U- 230Th, 235U- 231Pa and 230Th- 226Ra. This implies that, while large disequilibrium between 238U- 230Th and between 235U- 231Pa may occur together, large 230Th- 226Ra disequilibrium will not coexist with large 238U- 230Th disequilibrium, consistent with some observations. The active mantle melting zone which supplies melt to a ridge axis is inferred to be only about 10 km thick and 50 km wide. The fraction of melt present in such a mantle source at any time is about 0.01 and 0.04, respectively, if melting rate is 10 -7 and 10 -6 y -1. The corresponding residence time of the residual melt in the matrix is 10 5 and 4 × 10 4y.