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.
On the Nature of the Cherdyntsev-Chalov Effect
NASA Astrophysics Data System (ADS)
Timashev, S. F.
2018-06-01
It is shown that the Cherdyntsev-Chalov effect, usually presented as the separation of even isotopes of uranium upon their transition from the solid to the liquid phase, can include initiated acceleration of the radioactive decay of uranium-238 nuclei during the formation of cracks in geologically (seismic and volcanically) active zones of the Earth's crust. The fissuring of the solid-phase medium leads to an increase in mechanical tensile stress and the emergence of strong local electric fields, resulting in the injection of chemical-scale high-energy electrons into the aqueous phase of the cracks. Under these conditions, the e - catalytic decay of uranium-238 nucleus studied earlier can occur during the formation of metastable protactinium-238 nuclei with locally distorted nucleon structure, which subequently undergo β-decay with the formation of thorium-234 and helium-4 nuclei as products of the fission of the initial uranium-238 nucleus with a characteristic period of several years. The observed increased activity of uranium-234 nuclei that form during the subsequent β-decay of thorium and then protactinium is associated with the initiated fission of uranium-238. The possibility is discussed of developing thermal power by using existing wastes from uranium production that contain uranium-238 to activate this isotope through the mechanochemical processing of these wastes in aqueous media with the formation of 91 238 Pa isu , the half-life of which is several years.
Pérez-Sánchez, D; Thorne, M C
2014-05-01
In a previous paper, a mathematical model for the behaviour of (79)Se in soils and plants was described. Subsequently, a review has been published relating to the behaviour of (238)U-series radionuclides in soils and plants. Here, we bring together those two strands of work to describe a new mathematical model of the behaviour of (238)U-series radionuclides entering soils in solution and their uptake by plants. Initial studies with the model that are reported here demonstrate that it is a powerful tool for exploring the behaviour of this decay chain or subcomponents of it in soil-plant systems under different hydrological regimes. In particular, it permits studies of the degree to which secular equilibrium assumptions are appropriate when modelling this decay chain. Further studies will be undertaken and reported separately examining sensitivities of model results to input parameter values and also applying the model to sites contaminated with (238)U-series radionuclides. Copyright © 2013 Elsevier Ltd. All rights reserved.
Testing the concept of drift shadow at Yucca Mountain, Nevada
Paces, J.B.; Neymark, L.A.; Ghezzehei, T.; Dobson, P.F.
2006-01-01
If proven, the concept of drift shadow, a zone of reduced water content and slower ground-water travel time beneath openings in fractured rock of the unsaturated zone, may increase performance of a proposed geologic repository for high-level radioactive waste at Yucca Mountain, To test this concept under natural-flow conditions present in the proposed repository horizon, isotopes within the uranium-series decay chain (uranium-238, uranium-234, and thorium-230, or 238U-234U-230Th) have been analyzed in samples of rock from beneath four naturally occurring lithophysal cavities. All rock samples show 234U depletion relative to parent 238U indicating varying degrees of water-rock interaction over the past million years. Variations in 234U/238U activity ratios indicate that depletion of 234U relative to 238U can be either smaller or greater in rock beneath cavity floors relative to rock near cavity margins. These results are consistent with the concept of drift shadow and with numerical simulations of meter-scale spherical cavities in fractured tuff. Differences in distribution patterns of 234U/ 238U activity ratios in rock beneath the cavity floors are interpreted to reflect differences in the amount of past seepage into lithophysal cavities, as indicated by the abundance of secondary mineral deposits present on the cavity floors.
Measurement of the total activity concentrations of Libyan oil scale
NASA Astrophysics Data System (ADS)
Da Silva, F. C. A.; Bradley, D. A.; Regan, P. H.; Rozaila, Z. Siti
2017-08-01
Twenty-three oil scale samples obtained from the Libyan oil and gas industry production facilities onshore have been measured using high-resolution gamma-ray spectrometry with a shielded HPGe detector, the work being carried out within the Environmental Radioactivity Laboratory at the University of Surrey. The main objectives of this work were to determine the extent to which the predominant radionuclides associated with the uranium and thorium natural decay chains were in secular equilibrium with their decay progeny, also to compare differences between the total activity concentrations (TAC) in secular equilibrium and disequilibrium and to evaluate the measured activities for the predominant gamma-ray emitting decay radionuclides within the 232Th and 238U chains. The oil scale NORM samples did not exhibit radioactive equilibrium between the decay progeny and longer-lived parent radionuclides of the 238U and 232Th series.
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.
Disequilibrium in the uranium and actinium series in oil scale samples.
Landsberger, S; Tamalis, D; Leblanc, C; Yoho, M D
2017-01-01
We have investigated the disequilibrium of the uranium and actinium series and have found both 226 Ra (90,200 ± 4300 Bq/kg) and 228 Ra have activity concentrations orders of magnitude higher that 238 U (1.83 ± 0.36 Bq/kg) and 232 Th (7.0 ± 0.4) which are at the head of the decay series. As well the activity concentration of 210 Pb (24,400 ± 1200 Bg/kg) was about 3.6 times less than 226 Ra. Once an efficiency curve was constructed summing corrections for specific isotopes in the decay change also needed to be taken in consideration. Furthermore, self-attenuation of the photons especially the 46.5 keV belonging to 210 Pb was calculated to be 78% since the scale had elevated elemental concentrations of high-Z elements such as barium and strontium. Copyright © 2016 Elsevier Ltd. All rights reserved.
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
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.
Method for radioactivity monitoring
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.
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.
Sampling and analysis for radon-222 dissolved in ground water and surface water
DeWayne, Cecil L.; Gesell, T.F.
1992-01-01
Radon-222 is a naturally occurring radioactive gas in the uranium-238 decay series that has traditionally been called, simply, radon. The lung cancer risks associated with the inhalation of radon decay products have been well documented by epidemiological studies on populations of uranium miners. The realization that radon is a public health hazard has raised the need for sampling and analytical guidelines for field personnel. Several sampling and analytical methods are being used to document radon concentrations in ground water and surface water worldwide but no convenient, single set of guidelines is available. Three different sampling and analytical methods - bubbler, liquid scintillation, and field screening - are discussed in this paper. The bubbler and liquid scintillation methods have high accuracy and precision, and small analytical method detection limits of 0.2 and 10 pCi/l (picocuries per liter), respectively. The field screening method generally is used as a qualitative reconnaissance tool.
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 use of γ-rays analysis by HPGe detector to assess the gross alpha and beta activities in waters.
Casagrande, M F S; Bonotto, D M
2018-07-01
This paper describes an alternative method for evaluating gross alpha and beta radioactivity in waters by using γ-rays analysis performed with hyper-pure germanium detector (HPGe). Several gamma emissions related to α and β - decays were used to provide the activity concentration data due to natural radionuclides commonly present in waters like 40 K and those belonging to the 238 U and 232 Th decay series. The most suitable gamma emissions related to β - decays were 214 Bi (1120.29 keV, 238 U series) and 208 Tl (583.19 keV, 232 Th series) as the equation in activity concentration yielded values compatible to those generated by the formula taking into account the detection efficiency. The absence of isolated and intense γ-rays peaks associated to α decays limited the choice to 226 Ra (186.21 keV, 238 U series) and 224 Ra (240.99 keV, 232 Th series). In these cases, it was adopted appropriate correction factors involving the absolute intensities and specific activities for avoiding the interferences of other γ-rays energies. The critical level of detection across the 186-1461 keV energy region corresponded to 0.010, 0.023, 0.038, 0.086, and 0.042 Bq/L, respectively, for 226 Ra, 224 Ra, 208 Tl, 214 Bi and 40 K. It is much lower than the WHO guideline reference value for gross alpha (0.5 Bq/L) and beta (1.0 Bq/L) in waters. The method applicability was checked by the analysis of groundwater samples from different aquifer systems occurring in the Brazilian states of São Paulo, Minas Gerais and Mato Grosso do Sul. The waters exhibit very different chemical composition and the samples with the highest radioactivity levels were those associated with lithotypes possessing enhanced uranium and thorium levels. The technique allowed directly discard the 40 K contribution to the gross beta activity as potassium is an essential element for humans. Copyright © 2018 Elsevier Ltd. All rights reserved.
Gray, John R.; Fisk, Gregory G.
1992-01-01
From July 1988 through September 1991, radionuclide and suspended-sediment transport were monitored in ephemeral streams in the semiarid Little Colorado River basin of Arizona and New Mexico, USA, where in-stream gross-alpha plus gross-beta activities have exceeded Arizona's Maximum Allowable Limit through releases from natural weathering processes and from uranium-mining operations in the Church Rock Mining District, Grants Mineral Belt, New Mexico. Water samples were collected at a network of nine continuous-record streamgauges equipped with microprocessor-based satellite telemetry and automatic water-sampling systems, and six partial-record streamgauges equipped with passive water samplers. Analytical results from these samples were used to calculate transport of selected suspended and dissolved radionuclides in the uranium-238 and thorium-232 decay series.
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.
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.
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.
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.
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.
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.
Origin of uranium isotope variations in early solar nebula condensates.
Tissot, François L H; Dauphas, Nicolas; Grossman, Lawrence
2016-03-01
High-temperature condensates found in meteorites display uranium isotopic variations ((235)U/(238)U), which complicate dating the solar system's formation and whose origin remains mysterious. It is possible that these variations are due to the decay of the short-lived radionuclide (247)Cm (t 1/2 = 15.6 My) into (235)U, but they could also be due to uranium kinetic isotopic fractionation during condensation. We report uranium isotope measurements of meteoritic refractory inclusions that reveal excesses of (235)U reaching ~+6% relative to average solar system composition, which can only be due to the decay of (247)Cm. This allows us to constrain the (247)Cm/(235)U ratio at solar system formation to (1.1 ± 0.3) × 10(-4). This value provides new clues on the universality of the nucleosynthetic r-process of rapid neutron capture.
Limits on uranium and thorium bulk content in GERDA Phase I detectors
NASA Astrophysics Data System (ADS)
Collaboration, Gerda; Agostini, M.; Allardt, M.; Bakalyarov, A. M.; Balata, M.; Barabanov, I.; Baudis, L.; Bauer, C.; Becerici-Schmidt, N.; Bellotti, E.; Belogurov, S.; Belyaev, S. T.; Benato, G.; Bettini, A.; Bezrukov, L.; Bode, T.; Borowicz, D.; Brudanin, V.; Brugnera, R.; Caldwell, A.; Cattadori, C.; Chernogorov, A.; D'Andrea, V.; Demidova, E. V.; di Vacri, A.; Domula, A.; Doroshkevich, E.; Egorov, V.; Falkenstein, R.; Fedorova, O.; Freund, K.; Frodyma, N.; Gangapshev, A.; Garfagnini, A.; Grabmayr, P.; Gurentsov, V.; Gusev, K.; Hakemüller, J.; Hegai, A.; Heisel, M.; Hemmer, S.; Hofmann, W.; Hult, M.; Inzhechik, L. V.; Janicskó Csáthy, J.; Jochum, J.; Junker, M.; Kazalov, V.; Kihm, T.; Kirpichnikov, I. V.; Kirsch, A.; Kish, A.; Klimenko, A.; Kneißl, R.; Knöpfle, K. T.; Kochetov, O.; Kornoukhov, V. N.; Kuzminov, V. V.; Laubenstein, M.; Lazzaro, A.; Lebedev, V. I.; Lehnert, B.; Liao, H. Y.; Lindner, M.; Lippi, I.; Lubashevskiy, A.; Lubsandorzhiev, B.; Lutter, G.; Macolino, C.; Majorovits, B.; Maneschg, W.; Medinaceli, E.; Mingazheva, R.; Misiaszek, M.; Moseev, P.; Nemchenok, I.; Palioselitis, D.; Panas, K.; Pandola, L.; Pelczar, K.; Pullia, A.; Riboldi, S.; Rumyantseva, N.; Sada, C.; Salamida, F.; Salathe, M.; Schmitt, C.; Schneider, B.; Schönert, S.; Schreiner, J.; Schütz, A.-K.; Schulz, O.; Schwingenheuer, B.; Selivanenko, O.; Shevchik, E.; Shirchenko, M.; Simgen, H.; Smolnikov, A.; Stanco, L.; Stepaniuk, M.; Vanhoefer, L.; Vasenko, A. A.; Veresnikova, A.; von Sturm, K.; Wagner, V.; Walter, M.; Wegmann, A.; Wester, T.; Wiesinger, C.; Wojcik, M.; Yanovich, E.; Zhitnikov, I.; Zhukov, S. V.; Zinatulina, D.; Zuber, K.; Zuzel, G.
2017-05-01
Internal contaminations of 238U, 235U and 232Th in the bulk of high purity germanium detectors are potential backgrounds for experiments searching for neutrinoless double beta decay of 76Ge. The data from GERDA Phase I have been analyzed for alpha events from the decay chain of these contaminations by looking for full decay chains and for time correlations between successive decays in the same detector. No candidate events for a full chain have been found. Upper limits on the activities in the range of a few nBq/kg for 226Ra, 227Ac and 228Th, the long-lived daughter nuclides of 238U, 235U and 232Th, respectively, have been derived. With these upper limits a background index in the energy region of interest from 226Ra and 228Th contamination is estimated which satisfies the prerequisites of a future ton scale germanium double beta decay experiment.
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.
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.
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.
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
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
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
Colmenero Sujo, L; Montero Cabrera, M E; Villalba, L; Rentería Villalobos, M; Torres Moye, E; García León, M; García-Tenorio, R; Mireles García, F; Herrera Peraza, E F; Sánchez Aroche, D
2004-01-01
High-resolution gamma spectrometry was used to determine the concentration of 40K, 238U and 232Th series in soil samples taken from areas surrounding the city of Aldama, in Chihuahua. Results of indoor air short-time sampling, with diffusion barrier charcoal detectors, revealed relatively high indoor radon levels, ranging from 29 to 422 Bq/m3; the radon concentrations detected exceeded 148 Bq/m3 in 76% of the homes tested. Additionally, liquid scintillation counting showed concentrations of radon in drinking water ranging from 4.3 to 42 kBq/m3. The high activity of 238U in soil found in some places may be a result of the uranium milling process performed 20 years ago in the area. High radon concentrations indoor and in water may be explained by assuming the presence of uranium-bearing rocks underneath of the city, similar to a felsic dike located near Aldama. The estimated annual effective dose of gamma radiation from the soil and radon inhalation was 3.83 mSv.
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.
ERIC Educational Resources Information Center
Alexander, John J., Ed.
1978-01-01
Two exam questions are presented. One suitable for advanced undergraduate or beginning graduate courses in organic chemistry, is on equivalent expressions for the description of several pericyclic reactions. The second, for general chemistry students, asks for an estimation of the rate of decay of a million-year-old Uranium-238 sample. (BB)
Characteristics of NORM in the oil industry from eastern and western deserts of Egypt.
Shawky, S; Amer, H; Nada, A A; El-Maksoud, T M; Ibrahiem, N M
2001-07-01
Naturally occurring radionuclides (NORs) from the 232Th- and 238U-series, which are omnipresent in the earth's crust, can be concentrated by technical activities, particularly those involving natural resources. Although, a great deal of work has been done in the field of radiation protection and remedial action on uranium and other mines, recent concern has been devoted to the hazard arising from naturally occurring radioactive materials (NORM) in oil and gas facilities. NORM wastes associated with oil and gas operations from scale deposits, separated sludge and water at different oil fields in the eastern and western deserts were investigated. Concentrations of the uranium, thorium, and potassium (40K) series have been determined from high-resolution gamma-ray spectrometry. Total uranium content of samples was determined using laser fluorimetry. The levels of radioactivity were mainly due to enhanced levels of dissolved radium ions. Only minute quantities of uranium and thorium were present. The disequilibrium factor for 238U/226Ra has been determined.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Marsh, S.F.; Spall, W.D.; Abernathey, R.M.
1976-11-01
Relationships are provided to compute the decreasing plutonium content and changing isotopic distribution of plutonium materials for the radioactive decay of /sup 238/Pu, /sup 239/Pu, /sup 240/Pu and /sup 242/Pu to long-lived uranium daughters and of /sup 241/Pu to /sup 241/Am. This computation is important to the use of plutonium reference materials to calibrate destructive and nondestructive methods for assay and isotopic measurements, as well as to accountability inventory calculations.
Assessing Natural Radionuclide Migration in the Legacy Tailings of Uranium Production
NASA Astrophysics Data System (ADS)
Bondarenko, G.; Koliabina, I.; Marinich, O.
2011-12-01
The former Prydniprovsky Chemical Plant in Dniprodzerzhynsk, Ukraine, processed uranium ore from 1949 until 1991. Multiple tailing ponds containing solid residual waste products from the uranium leaching and processing of uranium were accumulated along the Dnieper River, including the largest, adjacent to the Dnieper Reservoir, containing over 12 million tons of tailings. Samples for this study were selected from a core recovered from the Dnieper tailing pit in 2009, and used to assess radionuclide migration from tailing ponds. Samples were selected from different depths of the tailing pit core, analyzed for total radionuclide concentrations [Marinich et al., 2009], and successively leached using distilled water, followed by 1N ammonium acetate solution, and finally by 1N HCl solution. Leaching times were ~24 h at 15.17 °C. 238U, 230Th and 226Ra leachate activities were measured by γ-spectrometry with a Ge(Li) detector. 210Pb activity was measured using a SEB-01 scintillation β-spectrometer. Errors depended on measuring method, radionuclide, activity and exposure time: 238U, 11.9%; 230Th, 10.9%; 226Ra, 9.3%; 210Pb ~30%. The average total 238U activity in the tailing profile was 4 Bq/g. The concentration of 238U in the water leachates increased with depth from 14.5% (7-7.5 m), to 43% (11-11.5 m). The concentration of 238U in the acid leachates behaved similarly, increasing from 5.5 % to 15.5% with depth. While the total 230Th activity in increased from 30 Bq/g (7-7.5 m) to 540 Bq/g (11-11.5 m), the 230Th concentration in ammonium acetate leachates decreased from ˜15% to ˜1%. The concentration of 226Ra in all leachates was <1%, indicating that, under conditions of the Dnieper tailing pit, 226Ra is essentially immobile. The concentration of 210Pb in the leachates was as high as 10%. In general, the magnitude of mobile activity from the Dnieper tailing pit core samples decreases in the order 238U>230Th≥210Pb> 226Ra. Secular radioactive equilibrium in the 238U - 230Th - 226Ra - 210Pb decay chain, typical for closed systems, has been disturbed during selective chemical uranium extraction from the parent ore. We calculated the migration of 210Pb, assuming constant 226Ra activity. The results of these calculations show that over 50 years, ~18% of the initial (unknown) 210Pb(0) activity was removed. If we assume removal of 226Ra decay products will continue at the current level, we expect the future annual activity loss of 210Pb to be about 0.36% per year, or 0.072 Bq/g. Assuming the examined core sample is representative of all 12 million tons of tails, the total annual activity loss is estimated to be ~1012 Bq/year. These results allow us to conclude that the loss of activity from the tailing pit by water migration is mainly associated with the 226Ra decay products: 222Rn, 210Pb, 210Po.
Activity ratios, Dnieper tailings
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.
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
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.
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.
NASA Astrophysics Data System (ADS)
Uvarova, Yulia A.; Kyser, T. Kurt; Geagea, Majdi Lahd; Chipley, Don
2014-12-01
Variations in 238U/235U and 234U/238U ratios were measured in uranium minerals from a spectrum of uranium deposit types, as well as diagenetic phosphates in uranium-rich basins and peraluminous rhyolites and associated autunite mineralisation from Macusani Meseta, Peru. Mean δ238U values of uranium minerals relative to NBL CRM 112-A are 0.02‰ for metasomatic deposits, 0.16‰ for intrusive, 0.18‰ for calcrete, 0.18‰ for volcanic, 0.29‰ for quartz-pebble conglomerate, 0.29‰ for sandstone-hosted, 0.44‰ for unconformity-type, and 0.56‰ for vein, with a total range in δ238U values from -0.30‰ to 1.52‰. Uranium mineralisation associated with igneous systems, including low-temperature calcretes that are sourced from U-rich minerals in igneous systems, have low δ238U values of ca. 0.1‰, near those of their igneous sources, whereas uranium minerals in basin-hosted deposits have higher and more variable values. High-grade unconformity-related deposits have δ238U values around 0.2‰, whereas lower grade unconformity-type deposits in the Athabasca, Kombolgie and Otish basins have higher δ238U values. The δ234U values for most samples are around 0‰, in secular equilibrium, but some samples have δ234U values much lower or higher than 0‰ associated with addition or removal of 234U during the past 2.5 Ma. These δ238U and δ234U values suggest that there are at least two different mechanisms responsible for 238U/235U and 234U/238U variations. The 234U/238U disequilibria ratios indicate recent fluid interaction with the uranium minerals and preferential migration of 234U. Fractionation between 235U and 238U is a result of nuclear-field effects with enrichment of 238U in the reduced insoluble species (mostly UO2) and 235U in oxidised mobile species as uranyl ion, UO22+, and its complexes. Therefore, isotopic fractionation effects should be reflected in 238U/235U ratios in uranium ore minerals formed either by reduction of uranium to UO2 or chemical precipitation in the form of U6+ minerals. The δ238U values of uranium ore minerals from a variety of deposits are controlled by the isotopic signature of the uranium source, the efficiency of uranium reduction in the case of UO2 systems, and the degree to which uranium was previously removed from the fluid, with less influence from temperature of ore formation and later alteration of the ore. Uranium isotopes are potentially superb tracers of redox in natural systems.
Modification of apparent fission yields by Chemical Fractionation following Fission (CFF)
NASA Astrophysics Data System (ADS)
Hohenberg, Charles; Meshik, Alex
2008-04-01
Grain-by-grain studies of the 2 billion year old Oklo natural reactor, using laser micro-extraction^1,2, yield detailed information about Oklo, a water-moderated pulsed reactor, cycle times, total neutron fluence and duration, but it also demonstrates Chemical Fractionation following Fission. In the CFF process, members of an isobaric yield chain with long half-lives are subject to migration before decay can occur. Of particular interest is the 129 isobar where 17 million ^129I can migrate out of the host grain before decay, and iodine compounds are water soluble. This is amply demonstated by the variation of Xe spectra between micron-sized uranium-bearing minerals and adjacent uranium-free minerals. Fission 129 yields for the spontaneous fission of ^238U generally come from measured ^129Xe in pitchblend^2, ores emplaced by aqueous activity, and are incorrect due to the CFF process. ^238U yields for the 131 and 129 chains, reported in Hyde^3, as 0.455 +- .02 and < 0.012, respectively, the latter being anomalously low. ^1A Meshik, C Hohenberg and O Pravdivtesva, PRL 93, 182302 (2004); A Meshik Sci. Am. Nov (2005), 55; ^2E K Hyde, Nucl Prop of Heavy Elements III (1964).
Radioisotope dilution analyses of geological samples using 236U and 229Th
Rosholt, J.N.
1984-01-01
The use of 236U and 229Th in alpha spectrometric measurements has some advantages over the use of other tracers and measurement techniques in isotope dilution analyses of most geological samples. The advantages are: (1) these isotopes do not occur in terrestrial rocks, (2) they have negligible decay losses because of their long half lives, (3) they cause minimal recoil contamination to surface-barrier detectors, (4) they allow for simultaneous determination of the concentration and isotopic composition of uranium and thorium in a variety of sample types, and (5) they allow for simple and constant corrections for spectral inferences, 0.5% of the 238U activity is subtracted for the contribution of 235U in the 236U peak and 1% of the 229Th activity is subtracted from the 230Th activity. Disadvantages in using 236U and 229Th are: (1) individual separates of uranium and thorium must be prepared as very thin sources for alpha spectrometry, (2) good resolution in the spectrometer system is required for thorium isotopic measurements where measurement times may extend to 300 h, and (3) separate calibrations of the 236U and 229Th spike solution with both uranium and thorium standards are required. The use of these tracers in applications of uranium-series disequilibrium studies has simplified the measurements required for the determination of the isotopic composition of uranium and thorium because of the minimal corrections needed for alpha spectral interferences. ?? 1984.
Concentration of Uranium Radioisotopes in Albanian Drinking Waters Measured by Alpha Spectrometry
NASA Astrophysics Data System (ADS)
Bylyku, Elida; Cfarku, Florinda; Deda, Antoneta; Bode, Kozeta; Fishka, Kujtim
2010-01-01
Uranium is a radioactive material that is frequently found in rocks and soil. When uranium decays, it changes into different elements that are also radioactive, including radon, a gas that is known to cause a lung cancer. The main concern with uranium in drinking water is harm to the kidneys. Public water systems are required to keep uranium levels at or below 500 mBq per liter to protect against kidney damage. Such an interest is needed due to safety, regulatory compliance and disposal issue for uranium in the environment since uranium is included as an obligatory controlled radionuclide in the European Legislation (Directive 98/83 CE of Council of 03.11.1998). The aim of this work is to measure the levels of uranium in drinking and drilled well waters in Albania. At first each sample was measured for total Alpha and total Beta activity. The samples with the highest levels of total alpha activity were chosen for the determination of uranium radioisotopes by alpha spectrometry. A radiochemical procedure using extraction with TBP (Tri-Butyl-Phosphate) is used in the presence of U232 as a yield tracer. Thin sources for alpha spectrometry are prepared by electrodepositing on to stainless steel discs. The results of the U238 activity measured in the different samples, depending from their geological origin range between 0.55-13.87 mBq/l. All samples measured results under the European Directive limits for U238 (5-500 mBq/1), Dose Coefficients according to Directive 96/29 EURATOM.
Rapid Method for Sodium Hydroxide Fusion of Concrete and ...
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hoppe, Eric W.; Aalseth, Craig E.; Brodzinski, Ronald L.
The search for neutrinoless double beta decay in 76Ge has driven the need for ultra-low background Ge detectors shielded by electroformed copper of ultra-high radiopurity (<0.1µBq/kg). Although electrodeposition processes are almost sophisticated enough to produce copper of this purity, to date there are no methods sensitive enough to assay it. Inductively-coupled plasma mass spectrometry (ICP/MS) can detect thorium and uranium at femtogram levels, but in the past, this assay has been hindered by high copper concentrations in the sample. Electrodeposition of copper samples removes copper from the solution while selectively concentrating thorium and uranium contaminants to be assayed by ICP/MS.more » Spiking 232Th and 238U into the plating bath simulates low purity copper and allows for the calculation of the electrochemical rejection rate of thorium and uranium in the electroplating system. This rejection value will help to model plating bath chemistry.« less
An Empirical Method for Determining 234U Percentage
DOE Office of Scientific and Technical Information (OSTI.GOV)
Miko, David K.
2015-11-02
When isotopic information for uranium is provided, the concentration of 234U is frequently neglected. Often the isotopic content is given as a percentage of 235U with the assumption that the remainder consists of 238U. In certain applications, such as heat output, the concentration of 234U can be a significant contributing factor. For situations where only the 235U and 238U values are given, a simple way to calculate the 234U component would be beneficial. The approach taken here is empirical. A series of uranium standards with varying enrichments were analyzed. The 234U and 235U data were fit using a second ordermore » polynomial.« less
Rapid Method for Sodium Hydroxide Fusion of Asphalt ...
Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 Rapid method developed for analysis of Americium-241 (241Am), plutonium-238 (238Pu), plutonium-239 (239Pu), radium-226 (226Ra), strontium-90 (90Sr), uranium-234 (234U), uranium-235 (235U) and uranium-238 (238U) in asphalt roofing material samples
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reinitz, I.M.; Turekian, K.K.
1991-12-01
The concentrations of members of the {sup 238}U decay chain and {sup 232}Th have been determined for the lavas that erupted on the East Rift Zone of Kilauea Volcano, Hawaii (Puu Oo) between January 1983 and January 1985. There was a decrease during the first 180 days in the abundances of all nuclides, following the behavior of the incompatible elements. ({sup 230}Th/{sup 238}U) varies with ({sup 232}Th/{sup 238}U) yielding a batch process age for the source magma of 127,800 {plus minus} 28,500 (2{omega}) y, similar to East Pacific Rise basalts. No ({sup 226}Ra/{sup 230}Th) disequilibrium was evident at Puu Oomore » although Haleakala and Loihi show significant excesses of ({sup 226}Ra) over ({sup 230}Th). The initial ({sup 210}Pb) excess relative to ({sup 226}Ra) implies strong incompatibility of {sup 210}Pb probably with the help of chloride complexing, and the deficiency in later episodes indicates volatilization from the melt mediated by the formation of volatile chloride compounds.« less
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
Polonium-210 accumulates in a lake receiving coal mine discharges-anthropogenic or natural?
Nelson, A W; Eitrheim, E S; Knight, A W; May, D; Wichman, M D; Forbes, T Z; Schultz, M K
2017-02-01
Coal is an integral part of global energy production; however, coal mining is associated with numerous environmental health impacts. It is well documented that coal-mine waste can contaminate the environment with naturally-occurring radionuclides from the uranium-238 ( 238 U) decay series. However, the behavior of the final radionuclide in the 238 U-series, i.e., polonium-210 ( 210 Po) arising from coal-mine waste-water discharge is largely unexplored. Here, results of a year-long (2014-2015) field study, in which the concentrations of 210 Po in sediments and surface water of a lake that receives coal-mine waste-water discharge in West Virginia are presented. Initial measurements identified levels of 210 Po in the lake sediments that were in excess of that which could be attributed to ambient U-series parent radionuclides; and were indicative of discharge site contamination of the lake ecosystem. However, control sediment obtained from a similar lake system in Iowa (an area with no coal mining or unconventional drilling) suggests that the levels of 210 Po in the lake are a natural phenomenon; and are likely unrelated to waste-water treatment discharges. Elevated levels of 210 Po have been reported in lake bottom sediments previously, yet very little information is available on the radioecological implications of 210 Po accumulation in lake bottom sediments. The findings of this study suggest that (Monthly Energy Review, 2016) the natural accumulation and retention of 210 Po in lake sediments may be a greater than previously considered (Chadwick et al., 2013) careful selection of control sites is important to prevent the inappropriate attribution of elevated levels of NORM in lake bottom ecosystems to industrial sources; and (Van Hook, 1979) further investigation of the source-terms and potential impacts on elevated 210 Po in lake-sediment ecosystems is warranted. Copyright © 2016 Elsevier Ltd. All rights reserved.
Forte, M; Rusconi, R; Margini, C; Abbate, G; Maltese, S; Badalamenti, P; Bellinzona, S
2001-01-01
The uranium concentration in 59 samples of bottled and tap water, mainly from northern Italy, was measured by different techniques. Results obtained by inductively coupled plasma mass spectrometry (ICP-MS), semiconductor alpha spectrometry and low level liquid scintillation counting with alpha/beta discrimination (LSC) have been compared. High resolution gamma spectrometry and semiconductor alpha spectrometry have been used to analyse uranium in a variety of organic and inorganic samples. Isotopic secular equilibrium in the 238U series may be lacking or hidden by auto-absorption phenomena, so caution should be used in evaluating gamma spectrometry data. Alpha spectrometry has also been used to ascertain the possible pollution from depleted uranium in the environment.
Zhou, Juanzuo; Lundstrom, C.C.; Fouke, B.; Panno, S.; Hackley, K.; Curry, B.
2005-01-01
Natural waters universally show fractionation of uranium series (U-series) parent-daughter pairs, with the disequilibrium between 234U and 238U (234U)/(238U) commonly used as a tracer of groundwater flow. Because speleothems provide a temporal record of geochemical variations in groundwater precipitating calcite, (234U)/(238U) variations in speleothems provide a unique method of investigating water-rock interaction processes over millennium time scales. We present high precision Thermal Ionization Mass Spectrometric (TIMS) U-series analyses of speleothems and drip waters from Fogelpole Cave in southern Illinois. Data from all speleothems from the cave show an inverse correlation between (234U)/(238U) and U concentration, following the pattern observed in groundwaters globally. Within a 65-cm-long stalagmite, concordant 234U-238 U-230Th and 235U-231Pa ages for 5 samples indicate accurate chronology from 78.5 ka to 30 ka. Notably, (234U)/(238U)o which differs from most speleothems by having (234U)/(238U)o <1, positively correlates with speleothem growth rate. We generalize this to the observation that speleothems globally show (234U)/ (238U)o deviating farther from secular equilibrium at lower growth rates and approaching secular equilibrium at higher grow rates. Based on the Fogelpole observations, we suggest that groundwater (234U)/(238U) is controlled by the U oxidation state, the U concentration of the water and the fluid velocity. A transport model whereby U-series nuclides react and exchange with mineral surfaces can reproduce the observed trend between growth rate and (234U)/(238U)o. Based on this result, we suggest that (234U)/(238U)o in speleothems may record changes in hydrologic flux with time and thus could provide a useful proxy for long term records of paleoprecipitation. ?? 2005 Elsevier B.V. All rights reserved.
Code of Federal Regulations, 2010 CFR
2010-07-01
... 40 Protection of Environment 1 2010-07-01 2010-07-01 false Timing of Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. 23.8 Section 23.8 Protection of Environment... Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. Unless the Administrator...
Code of Federal Regulations, 2013 CFR
2013-07-01
... 40 Protection of Environment 1 2013-07-01 2013-07-01 false Timing of Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. 23.8 Section 23.8 Protection of Environment... Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. Unless the Administrator...
Code of Federal Regulations, 2014 CFR
2014-07-01
... 40 Protection of Environment 1 2014-07-01 2014-07-01 false Timing of Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. 23.8 Section 23.8 Protection of Environment... Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. Unless the Administrator...
Code of Federal Regulations, 2012 CFR
2012-07-01
... 40 Protection of Environment 1 2012-07-01 2012-07-01 false Timing of Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. 23.8 Section 23.8 Protection of Environment... Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. Unless the Administrator...
Code of Federal Regulations, 2011 CFR
2011-07-01
... 40 Protection of Environment 1 2011-07-01 2011-07-01 false Timing of Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. 23.8 Section 23.8 Protection of Environment... Administrator's action under Uranium Mill Tailings Radiation Control Act of 1978. Unless the Administrator...
Modern Measurements of Uranium Decay Rates
NASA Astrophysics Data System (ADS)
Parsons-Moss, T.; Faye, S. A.; Williams, R. W.; Wang, T. F.; Renne, P. R.; Mundil, R.; Harrison, M.; Bandong, B. B.; Moody, K.; Knight, K. B.
2015-12-01
It has been widely recognized that accurate and precise decay constants (λ) are critical to geochronology as highlighted by the EARTHTIME initiative, particularly the calibration benchmarks λ235U and λ238U. [1] Alpha counting experiments in 1971[2] measured λ235U and λ238U with ~0.1% precision, but have never been independently validated. We are embarking on new direct measurements of λ235U, λ238U, λ234Th, and λ234U using independent approaches for each nuclide. For the measurement of λ235U, highly enriched 235U samples will be chemically purified and analyzed for U concentration and isotopic composition by multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Thin films will be electrodeposited from these solutions and the α activity will be measured in an α-γ coincidence counting apparatus, which allows reduced uncertainty in counting efficiency while achieving adequate counting statistics. For λ238U measurement we will measure ingrowth of 234Th in chemically purified, isotopically enriched 238U solutions, by quantitatively separating the Th and allowing complete decay to 234U. All of the measurements will be done using MC-ICP-MS aiming at 0.05% precision. This approach is expected to result in values of λ238U with less than 0.1% uncertainty, if combined with improved λ234Th measements. These will be achieved using direct decay measurements with an E-ΔE charged particle telescope in coincidence with a gamma detector. This system allows measurement of 234Th β-decay and simultaneous detection and identification of α particles emitted by the 234U daughter, thus observing λ234U at the same time. The high-precision λ234U obtained by the direct activity measurements can independently verify the commonly used values obtained by indirect methods.[3] An overarching goal of the project is to ensure the quality of results including metrological traceability in order to facilitate implementation across diverse disciplines. [1] T.M. Harrison et al., (2015) It's About Time:Opportunities and Challenges for U.S. Geological Survey. Institute of Geophysics and Planetary Physics Publication 6539, University of California, Los Angeles [2] A. H. Jaffey et al., Physical Review C, 4, 5, (1971), 1889-1906 [3] H. Cheng et al., Chemical Geology, 169, (2000), 17-33
Rapid Radiochemical Method for Isotopic Uranium in Building ...
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.
Yoho, Michael; Porterfield, Donivan R.; Landsberger, Sheldon
2015-09-22
In this study, twenty-one high purity germanium (HPGe) background spectra were collected over 2 years at Los Alamos National Laboratory. A quality assurance methodology was developed to monitor spectral background levels from thermal and fast neutron flux levels and naturally occurring radioactive material decay series radionuclides. 238U decay products above 222Rn demonstrated minimal temporal variability beyond that expected from counting statistics. 238U and 232Th progeny below Rn gas displayed at most twice the expected variability. Further, an analysis of the 139 keV 74Ge(n, γ) and 691 keV 72Ge(n, n') spectral features demonstrated temporal stability for both thermal and fastmore » neutron fluxes.« less
NASA Astrophysics Data System (ADS)
Sakata, S.; Hirakawa, S.; Iwano, H.; Danhara, T.; Hirata, T.
2014-12-01
Zircon U-Th-Pb dating method is one of the most important tools for estimating the duration of magmatism by means of coupling of uranium, actinium and thorium decay series. Using U-Pb dating method, its reliability is principally guaranteed by the concordance between 238U-206Pb and 235U-207Pb ages. In case of dating Quaternary zircons, however, the initial disequilibrium effect on 230Th and 231Pa should be considered. On the other hands, 232Th-208Pb dating method can be a simple but powerful approach for investigating the age of crystallization because of negligible influence from initial disequilibrium effect. We have developed a new correction model for accurate U-Pb dating of the young zircon samples by taking into consideration of initial disequilibrium and a U-Pb vs Th-Pb concordia diagram for reliable age calibration was successfully established. Hence, the U-Th-Pb dating method can be applied to various zircons ranging from Hadean (4,600 Ma) to Quaternary (~50 ka) ages, and this suggests that further detailed information concerning the thermal history of the geological sequences can be made by the coupling of U-Th-Pb, fission track and Ar-Ar ages. In this presentation, we will show an example of U-Th-Pb dating for zircon samples from Sambe Volcano (3 to 100 ka), southwest Japan and the present dating technique using LA-ICP-MS.
Rapid Method for Sodium Hydroxide Fusion of Asphalt ...
Technical Brief--Addendum to Selected Analytical Methods (SAM) 2012 The method will be used for qualitative analysis of americium-241, plutonium-238, plutonium-239, radium-226, strontium-90, uranium-234, uranium-235 and uranium-238 in asphalt matrices samples.
Potential effects of alpha-recoil on uranium-series dating of calcrete
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.
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.
Preliminary results from the lunar prospector alpha particle spectrometer
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lawson, S. L.
2001-01-01
The Lunar Prospector Alpha Particle Spectrometer (LP APS) builds on Apollo heritage and maps the distribution of outgassing sites on the Moon. The APS searches for lunar surface gas release events and maps their distribution by detecting alpha particles produced by the decay of gaseous radon-222 (5.5 MeV, 3.8 day half-life) and solid polonium-210 (5.3 MeV, 138 day half-life, but remains on the surface with a 21 year half-life as lead-210), which are radioactive daughters from the decay of uranium-238. Radon is in such small quantities that it is not released directly from the lunar interior, rather it is entrainedmore » in a stream of gases and serves as a tracer for such gases. Once released, the radon spreads out by 'bouncing' across the surface on ballistic trajectories in a random-walk process. The 3.8 day half-life of radon-222 allows the gas to spread out by several 100 km before it decays and allows the APS to detect gas release events up to a few days after they occur. The long residence time (10s of years) of the lead-210 precursor to the polonium-210 allows the mapping of gas vents which have been active over the last approximately 50 years. Because radon and polonium are daughter products of the decay of uranium, the background level of alpha particle activity is a function of the lunar crustal uranium distribution. Using radioactive radon and polonium as tracers, the Apollo 15 and 16 Command Module orbital alpha particle experiments obtained evidence for the release of gases at several sites beneath the orbit tracks, especially over the Aristarchus Plateau and Mare Fecunditatis [1]. Aristarchus crater had previously been identified by ground-based observers as the site of transient optical events [2]. The Apollo 17 surface mass spectrometer showed that argon-40 is released from the lunar interior every few months, apparently in concert with some of the shallow moonquakes that are believed to be of tectonic origin [3]. The latter tectonic events could be associated with very young scarps identified in the lunar highlands [4] and are believed to indicate continued global contraction. Such quakes could open fissures leading to the release of gases that are trapped below the surface. The detection of radon-222 outgassing events at the margins of Fecunditatis basin was surprising because the observed surface distribution of uranium and thorium do not extend sufficiently eastward to cover Fecunditatis. If the Apollo detections prove sound, then those alpha particle emissions indicate substantial subsurface concentrations of uranium-238 within Fecunditatis. A primary goal of the APS was to map gas-release events, thus allowing both an appraisal of the current level of tectonic activity on the Moon and providing a probe of subsurface uranium concentrations.« less
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.
Dissolution behaviour of 238U, 234U and 230Th deposited on filters from personal dosemeters.
Becková, Vera; Malátová, Irena
2008-01-01
Kinetics of dissolution of (238)U, (234)U and (230)Th dust deposited on filters from personal alpha dosemeters was studied by means of a 26-d in vitro dissolution test with a serum ultrafiltrate simulant. Dosemeters had been used by miners at the uranium mine 'Dolní Rozínka' at Rozná, Czech Republic. The sampling flow-rate as declared by the producer is 4 l h(-1) and the sampling period is typically 1 month. Studied filters contained 125 +/- 6 mBq (238)U in equilibrium with (234)U and (230)Th; no (232)Th series nuclides were found. Half-time of rapid dissolution of 1.4 d for (238)U and (234)U and slow dissolution half-times of 173 and 116 d were found for (238)U and (234)U, respectively. No detectable dissolution of (230)Th was found.
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
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
Natural Radiation from Soil using Gamma-Ray Spectrometry
DOE Office of Scientific and Technical Information (OSTI.GOV)
Silveira, M. A. G.; Moreira, R. H.; Paula, A. L. C. de
2009-06-03
We have studied the distribution of natural radioactivity in the soil of Interlagos, in Sao Paulo city and Billings Reservoir, in Sao Bernardo do Campo, Sao Paulo, Brazil. The main contribution of the effective radiation dose is due to the elements of the {sup 238}Th decay series, with smaller contributions from {sup 40}K and the elements of the series of {sup 238}U. The results indicate the dose in all of the studied areas is around the average international dose due to external exposure to gamma rays (0.48 mSv/yr) proceeding from natural terrestrial elements.
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
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.
Vector representation as a tool for detecting characteristic uranium peaks
NASA Astrophysics Data System (ADS)
Forney, Anne Marie
Vector representation is found as a viable tool for identifying the presence of and determining the difference between enriched and naturally occurring uranium. This was accomplished through the isolation of two regions of interest around the uranium-235 (235U) gamma emission at 186 keV and the uranium-238 (238U) gamma emission at 1001 keV. The uranium 186 keV peak is used as a meter for uranium enrichment, and events from this emission occurred more frequently with the increase of the 235U composition. Spectra were taken with the use of a high purity germanium detector in series with a multi-channel analyzer (MCA) and Maestro 32, a MCA emulator and spectral software. The vector representation method was used to compare two spectra by taking their dot product. The output from this method is an angle, which represents the similarity and contrast between the two spectra. When the angle is close to zero the spectra are similar, and as the angle approaches 90 degrees the spectral agreement decreases. The angles were calculated and compared in Microsoft Excel. A 49 % enriched uranyl acetate source containing both gamma emissions from 235U and 238U was used as a reference source to which all spectra were compared. Two other uranium sources were used within this project: a 100.2 nCi highly-enriched uranium source with 97.7 % 235U by weight, and a piece of uranium ore with an approximate exposure rate of 0.2 mR/h (51.5 nC/kg/h) at 1 cm. These two uranium sources provided different ratios of 235U to 238U, leading to different ratios of the 186 keV and 1001 keV peaks. To test the limits of the vector representation method, various source configurations were used. These included placing the source directly on top of the detector, using two distances for the source from the detector, using the source in addition to cobalt-60, and finally two distances for the source from the detector with a one centimeter lead shield. The two distances from the detector without the shielding were 1.3 inches (3.30 cm) and 1 foot (30.48 cm). In the cases using lead shielding, in the first geometry, the source was placed directly on the lead shielding and in the second geometry, the source was placed a foot above the lead shielding and detector. Vector representation output angles higher than a value of 40.3 degrees indicated that uranium was not present in the source. All of the sources tested with an angle below this 40.3 degree cutoff contained some type of uranium. To determine whether the uranium was processed or naturally occurring, 18.0 degrees was chosen as the upper limit for processed uranium sources. Sources that produced an angle above 18.0 degrees and below 40.3 degrees were categorized as naturally occurring uranium. The vector representation technique was able to classify the uranium sources in all of the geometries except for the geometries that included the centimeter of lead.
Uranium series dating of human skeletal remains from the Del Mar and Sunnyvale sites, California
Bischoff, J.L.; Rosenbauer, R.J.
1981-01-01
Uranium series analyses of human bone samples from the Del Mar and Sunnyvale sites indicate ages of 11,000 and 8,300 years, respectively. The dates are supported by internal concordancy between thorium-230 and protactinium-231 decay systems. These ages are significantly younger than the estimates of 48,000 and 70,000 years based on amino acid racemization, and indicate that the individuals could derive from the population waves that came across the Bering Strait during the last sea-level low. Copyright ?? 1981 AAAS.
β-decay spectroscopy for the r-process nucleosynthesis
DOE Office of Scientific and Technical Information (OSTI.GOV)
Nishimura, Shunji; Collaboration: RIBF Decay Collaborations
2014-05-09
Series of decay spectroscopy experiments, utilizing of high-purity Ge detectors and double-sided silicon-strip detectors, have been conducted to harvest the decay properties of very exotic nuclei relevant to the r-process nucleosynthesis at the RIBF. The decay properties such as β-decay half-lives, low-lying states, β-delayed neutron emissions, isomeric states, and possibly Q{sub β} of the very neutron-rich nuclei are to be measured to give significant constraints in the uncertainties of nuclear properties for the r-process nucleosynthesis. Recent results of βγ spectroscopy study using in-flight fission of {sup 238}U-beam will be presented together with our future perspectives.
NASA Astrophysics Data System (ADS)
Grün, Rainer; Aubert, Maxime; Joannes-Boyau, Renaud; Moncel, Marie-Hélène
2008-11-01
We have mapped U ( 238U) and Th ( 232Th) elemental concentrations as well as U-series isotope distributions in a Neanderthal tooth from the Middle Palaeolithic site of Payre using laser ablation ICP-MS. The U-concentrations in an enamel section varied between 1 and 1500 ppb. The U-concentration maps show that U-migration through the external enamel surface is minute, the bulk of the uranium having migrated internally via the dentine into the enamel. The uranium migration and uptake is critically dependent on the mineralogical structure of the enamel. Increased U-concentrations are observed along lineaments, some of which are associated with cracks, and others may be related to intra-prismatic zones or structural weaknesses reaching from the dentine into the enamel. The uranium concentrations in the dentine vary between about 25,000 and 45,000 ppb. Our systematic mapping of U-concentration and U-series isotopes provides insight into the time domain of U-accumulation. Most of the uranium was accumulated in an early stage of burial, with some much later overprints. None of the uranium concentration and U-series profiles across the root of the tooth complied with a single stage diffusion-adsorption (D-A) model that is used for quality control in U-series dating of bones and teeth. Nevertheless, in the domains that yielded the oldest apparent U-series age estimates, U-leaching could be excluded. This means that the oldest apparent U-series ages of around 200 ka represent a minimum age for this Neanderthal specimen. This is in good agreement with independent age assessments (200-230 ka) for the archaeological layer, in which it was found. The Th elemental concentrations in the dental tissues were generally low (between about 1 and 20 ppb), and show little relationship with the nature of the tissue.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Aguilar-Arevalo, A.
We present measurements of radioactive contamination in the high-resistivity silicon charge-coupled devices (CCDs) used by the DAMIC experiment to search for dark matter particles. Novel analysis methods, which exploit the unique spatial resolution of CCDs, were developed to identify α and β particles. Uranium and thorium contamination in the CCD bulk was measured through α spectroscopy, with an upper limit on the 238U ( 232Th) decay rate of 5 (15) kg -1 d -1 at 95% CL. We also searched for pairs of spatially correlated electron tracks separated in time by up to tens of days, as expected from 32Simore » – 32P or 210Pb – 210Bi sequences of b decays. The decay rate of 32Si was found to be 80 +110 -65 (95% CI). An upper limit of ~35 kg -1 d -1 (95% CL) on the 210Pb decay rate was obtained independently by α spectroscopy and the β decay sequence search. Furthermore, these levels of radioactive contamination are sufficiently low for the successful operation of CCDs in the forthcoming 100 g DAMIC detector.« less
NASA Astrophysics Data System (ADS)
Messier, K. P.; Serre, M. L.
2015-12-01
Radon (222Rn) is a naturally occurring chemically inert, colorless, and odorless radioactive gas produced from the decay of uranium (238U), which is ubiquitous in rocks and soils worldwide. Exposure to 222Rn 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 222Rn with anisotropic geological and 238U based explanatory variables is developed, which helps elucidate the factors contributing to elevated 222Rn across North Carolina. Geological and uranium based variables are constructed in elliptical buffers surrounding each observation such that they capture the lateral geometric anisotropy present in groundwater 222Rn. Moreover, geological features are defined at three different geological spatial scales to allow the model to distinguish between large area and small area effects of geology on groundwater 222Rn. 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 222Rn across North Carolina including prediction uncertainty. The LUR-BME model of groundwater 222Rn results in a leave-one out cross-validation of 0.46 (Pearson correlation coefficient= 0.68), effectively predicting within the spatial covariance range. Modeled results of 222Rn concentrations show variability among Intrusive Felsic geological formations likely due to average bedrock 238U defined on the basis of overlying stream-sediment 238U concentrations that is a widely distributed consistently analyzed point-source data.
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.
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.
NASA Astrophysics Data System (ADS)
Mullakaev, A. I.; Khasanov, R. R.; Badrutdinov, O. R.; Kamaletdinov, I. R.
2018-05-01
The article investigates geochemical features of Permian (Cisuralian, Ufimian Stage and Biarmian, Kazanian Stage of the General Stratigraphic Scale of Russia) bituminous sands and sandstones located on the territory of the Volga-Ural oil and gas province (Republic of Tatarstan). Natural bitumens are extracted using thermal methods as deposits of high-viscosity oils. In the samples studied, the specific activity of natural radionuclides from the 238U (226Ra), 232Th, and 40K series was measured using gamma spectrometry. As a result of the precipitation of uranium and thorium and their subsequent decay, the accumulation of radium (226Ra and 228Ra) has been shown to occur in the bituminous substance. In the process of exploitation of bitumen-bearing rock deposits (as an oil fields) radium in the composition of a water-oil mixture can be extracted to the surface or deposited on sulfate barriers, while being concentrated on the walls of pipes and other equipment. This process requires increased attention to monitoring and inspection the environmental safety of the exploitation procedure.
Modern U-Pb chronometry of meteorites: advancing to higher time resolution reveals new problems
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.
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.
NASA Astrophysics Data System (ADS)
Barzakh, A. E.; Lhersonneau, G.; Batist, L. Kh.; Fedorov, D. V.; Ivanov, V. S.; Mezilev, K. A.; Molkanov, P. L.; Moroz, F. V.; Orlov, S. Yu.; Panteleev, V. N.; Volkov, Yu. M.; Alyakrinskiy, O.; Barbui, M.; Stroe, L.; Tecchio, L. B.
2011-05-01
The diffusion-effusion model has been used to analyse the release and yields of Fr and Cs isotopes from uranium carbide targets of very different thicknesses (6.3 and 148 g/cm2) bombarded by a 1 GeV proton beam. Release curves of several isotopes of the same element and production efficiency versus decay half-life are well fitted with the same set of parameters. Comparison of efficiencies for neutron-rich and neutron-deficient Cs isotopes enables separation of the contributions from the primary ( p + 238U) and secondary (n + 238U) reactions to the production of neutron-rich Cs isotopes. A rather simple calculation of the neutron contribution describes these data fairly well. The FLUKA code describes the primary and secondary-reaction contributions to the Cs isotopes production efficiencies for different targets quite well.
Depleted uranium analysis in blood by inductively coupled plasma mass spectrometry
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.
Determination of uranium in tap water by ICP-MS.
El Himri, M; Pastor, A; de la Guardia, M
2000-05-01
A fast and accurate procedure has been developed for the determination of uranium at microg L(-1) level in tap and mineral water. The method is based on the direct introduction of samples, without any chemical pre-treatment, into an inductively coupled plasma mass spectrometer (ICP-MS). Uranium was determined at the mass number 238 using Rh as internal standard. The method provides a limit of detection of 2 ng L(-1) and a good repeatability with relative standard deviation values (RSD) about 3% for five independent analyses of samples containing 73 microg L(-1) of uranium. Recovery percentage values found for the determination of uranium in spiked natural samples varied between 91% and 106%. Results obtained are comparable with those found by radiochemical methods for natural samples and of the same order for the certified content of a reference material, thus indicating the accuracy of the ICP-MS procedure without the need of using isotope dilution. A series of mineral and tap waters from different parts of Spain and Morocco were analysed.
Elemental analysis using natural gamma-ray spectroscopy
NASA Astrophysics Data System (ADS)
Aksoy, A.; Naqvi, A. A.; Khiari, F. Z.; Abujarad, F.; Al-Ohali, M.; Sumani, M.
1994-12-01
A gamma-ray spectroscopy setup has been recently established to measure the natural gamma-ray activity from potassium ( 40K), uranium ( 238U), and thorium ( 232Th) isotopes in rock samples of oil well-logs. The setup mainly consists of a shielded 135 cm 3 Hyper Pure Germanium (HPGe) detector, a 5 in. × 5 in. NaT(Tl) detector and a PC based data acquisition system. The core samples, with 70-100 g weight, have cylindrical geometry and are sealed such that radon gas from 238U decay would not escape from the sample. For room background subtraction, pure quartz samples identical to core samples were used. The sample is first counted with the HPGe detector to identify the elements through its characteristics gamma rays. Then the elemental concentration is determined by counting the sample with a NaI detector. In order to determine the absolute concentrations, the sample activity is compared with the activities of standards supplied by NIST and IAEA. The concentration of 238U and 232Th has been determined in ppm range with that of 40K in wt.%.
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.
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.
Minor actinide transmutation in thorium and uranium matrices in heavy water moderated reactors
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bhatti, Zaki; Hyland, B.; Edwards, G.W.R.
2013-07-01
The irradiation of Th{sup 232} breeds fewer of the problematic minor actinides (Np, Am, Cm) than the irradiation of U{sup 238}. This characteristic makes thorium an attractive potential matrix for the transmutation of these minor actinides, as these species can be transmuted without the creation of new actinides as is the case with a uranium fuel matrix. Minor actinides are the main contributors to long term decay heat and radiotoxicity of spent fuel, so reducing their concentration can greatly increase the capacity of a long term deep geological repository. Mixing minor actinides with thorium, three times more common in themore » Earth's crust than natural uranium, has the additional advantage of improving the sustainability of the fuel cycle. In this work, lattice cell calculations have been performed to determine the results of transmuting minor actinides from light water reactor spent fuel in a thorium matrix. 15-year-cooled group-extracted transuranic elements (Np, Pu, Am, Cm) from light water reactor (LWR) spent fuel were used as the fissile component in a thorium-based fuel in a heavy water moderated reactor (HWR). The minor actinide (MA) transmutation rates, spent fuel activity, decay heat and radiotoxicity, are compared with those obtained when the MA were mixed instead with natural uranium and taken to the same burnup. Each bundle contained a central pin containing a burnable neutron absorber whose initial concentration was adjusted to have the same reactivity response (in units of the delayed neutron fraction β) for coolant voiding as standard NU fuel. (authors)« less
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.
Radioactivity in wastes generated from shale gas exploration and production - North-Eastern Poland.
Jodłowski, Paweł; Macuda, Jan; Nowak, Jakub; Nguyen Dinh, Chau
2017-09-01
In the present study, the K-40, U-238, Ra-226, Pb-210, Ra-228 and Th-228 activity concentrations were measured in 64 samples of wastes generated from shale gas exploration in North-Eastern Poland. The measured samples consist of drill cuttings, solid phase of waste drilling muds, fracking fluids, return fracking fluids and waste proppants. The measured activity concentrations in solid samples vary in a wide range from 116 to around 1100 Bq/kg for K-40, from 14 to 393 Bq/kg for U-238, from 15 to 415 Bq/kg for Ra-226, from 12 to 391 Bq/kg for Pb-210, from a few Bq/kg to 516 Bq/kg for Ra-228 and from a few Bq/kg to 515 Bq/kg for Th-228. Excluding the waste proppants, the measured activity concentrations in solid samples oscillate around their worldwide average values in soil. In the case of the waste proppants, the activity concentrations of radionuclides from uranium and thorium decay series are significantly elevated and equal to several hundreds of Bq/kg but it is connected with the mineralogical composition of proppants. The significant enhancement of Ra-226 and Ra-228 activity concentrations after fracking process was observed in the case of return fracking fluids, but the radium isotopes content in these fluids is comparable with that in waste waters from copper and coal mines in Poland. Copyright © 2017 Elsevier Ltd. All rights reserved.
Spatially-Resolved Analyses of Aerodynamic Fallout from a Uranium-Fueled Nuclear Test
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
SAM lists this method for the qualitative determination of Americium-241, Radium-226, Plutonium-238, Plutonium-239 and isotopic uranium in drinking water samples using alpha spectrometry and radiostrontium using beta counting.
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.
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.
NASA Astrophysics Data System (ADS)
Larijani, Cyrus Kouroush
This thesis is based on the development of a radiochemical separation scheme capable of separating both 236gNp and 236Pu from a uranium target of natural isotopic composition ( 1 g uranium) and 200 MBq of fission decay products. The isobaric distribution of fission residues produced following the bombardment of a natural uranium target with a beam of 25 MeV protons has been evaluated. Decay analysis of thirteen isobarically distinct fission residues were carried out using high-resolution gamma-ray spectrometry at the UK National Physical Laboratory. Stoichiometric abundances were calculated via the determination of absolute activity concentrations associated with the longest-lived members of each isobaric chain. This technique was validated by computational modelling of likely sequential decay processes through an isobaric decay chain. The results were largely in agreement with previously published values for neutron bombardments on natural uranium at energies of 14 MeV. Higher relative yields of products with mass numbers A 110-130 were found, consistent with the increasing yield of these radionuclides as the bombarding energy is increased. Using literature values for the production cross-section for fusion of protons with uranium targets, it is estimated that an upper limit of approximately 250 Bq of activity from the 236Np ground state was produced in this experiment. Using a radiochemical separation scheme, Np and Pu fractions were separated from the produced fission decay products, with analyses of the target-based final reaction products made using Inductively Couple Plasma Mass Spectrometry (ICP-MS) and high-resolution alpha and gamma-ray spectrometry. In a separate research theme, reliable measurement of Naturally Occurring Radioactive Materials is of significance in order to comply with environmental regulations and for radiological protection purposes. The thesis describes the standardisation of three reference materials, namely Sand, Tuff and TiO2 which can serve as quality control materials to achieve traceability, method validation and instrument calibration. The sample preparation, material characterization via gamma, alpha and Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and the assignment of values for both the 4n Thorium and 4n + 2 Uranium decay series are presented.
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.
NASA Astrophysics Data System (ADS)
Bajoga, Abubakar D.
A study of natural radioactivity from ninety different soil samples across the state of Kuwait was carried out with a view to ascertain the level of natural and/or man-made radioactivity from that area. There has been some concern on the levels of NORM following the First Gulf War in which approximately 300 tons of depleted uranium shells were used and in particular, whether it has a significant impact in the surrounding environment. This study uses gamma-spectroscopy in a low background measuring system employing a high resolution Hyper-Pure Germanium detector. The calculated specific activity concentrations are determined for the radionuclides 226Ra, 214Pb, 214Bi and 228Ac, 212Pb, 208Tl following the decays of the primordial radionuclides 238U and 232Th, respectively. The analysis also includes evaluations for the 235U decay chain. In particular, the 186 keV doublet transition is used together with the activity concentration values established from the decays of 214Bi and 214Pb to establish the 226Ra and 235U specific activity concentrations, which can be used to estimate the 235U:238U isotopic ratios and compare to the accepted value for naturally occurring material of 1:138. Specific activity concentration values have also been determined for the 40K and the anthropogenic radionuclide 137Cs (from fallout) were detected within the same samples. Results of the activity concentration gives mean value of 16.99±0.21, 12.79±0.14, 333±37 and 2.18±0.11 Bq/kg for 238U, 232Th, 40K, and 137Cs, respectively. The associated radiological hazard indices from these samples were found to have mean values of 29.13±0.35 nG/hr, 60.20±0.68 Bq/kg, and 35.30±0.40 µSv/year for the dose rates, radium equivalent, and annual dose equivalent, respectively. Analysed results of elemental concentrations of Uranium, Thorium and Potassium were also determined, and were found to range from 0.96±0.02 ppm to 2.53±0.02 ppm, 2.26±0.04 ppm to 5.23±0.05 ppm and a mean value of 1.21±0.03 % for 40K for the northern region, respectively. Overall result indicates values within the world average range. The results obtained for the 235U:238U isotopic ratio gives a mean value of 0.0462, which is consistent with the presence of natural material from the measured location.
Aguilar-Arevalo, A.
2015-08-25
We present measurements of radioactive contamination in the high-resistivity silicon charge-coupled devices (CCDs) used by the DAMIC experiment to search for dark matter particles. Novel analysis methods, which exploit the unique spatial resolution of CCDs, were developed to identify α and β particles. Uranium and thorium contamination in the CCD bulk was measured through α spectroscopy, with an upper limit on the 238U ( 232Th) decay rate of 5 (15) kg -1 d -1 at 95% CL. We also searched for pairs of spatially correlated electron tracks separated in time by up to tens of days, as expected from 32Simore » – 32P or 210Pb – 210Bi sequences of b decays. The decay rate of 32Si was found to be 80 +110 -65 (95% CI). An upper limit of ~35 kg -1 d -1 (95% CL) on the 210Pb decay rate was obtained independently by α spectroscopy and the β decay sequence search. Furthermore, these levels of radioactive contamination are sufficiently low for the successful operation of CCDs in the forthcoming 100 g DAMIC detector.« less
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.
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.
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.
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.
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
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.
Activity disequilibrium between 234U and 238U isotopes in natural environment.
Boryło, Alicja; Skwarzec, Bogdan
The aim of this work was to calculate the values of the 234 U/ 238 U activity ratio in natural environment (water, sediments, Baltic organisms and marine birds from various regions of the southern Baltic Sea; river waters (the Vistula and the Oder River); plants and soils collected near phosphogypsum waste heap in Wiślinka (Northern Poland) and deer-like animals from Northern Poland. On the basis of the studies it was found that the most important processes of uranium geochemical migration in the southern Baltic Sea ecosystem are the sedimentation of suspended material and the vertical diffusion from the sediments into the bottom water. Considerable values of the 234 U/ 238 U are characterized for the Vistula and Oder Rivers and its tributaries. The values of the 234 U/ 238 U activity ratio in different tissues and organs of the Baltic organisms, sea birds and wild deer are varied. Such a large variation value of obtained activity ratios indicates different behavior of uranium isotopes in the tissues and organisms of sea birds and wild animals. This value shows that uranium isotopes can be disposed at a slower or faster rate. The values of the 234 U/ 238 U activity ratio in the analyzed plants, soils and mosses collected in the vicinity of phosphogypsum dumps in Wiślinka are close to one and indicate the phosphogypsum origin of the analyzed nuclides. Uranium isotopes 234 U and 238 U are not present in radioactive equilibrium in the aquatic environment, which indicates that their activities are not equal. The inverse relationship is observed in the terrestrial environment, where the value of the of the 234 U/ 238 U activity ratio really oscillates around unity.
Searching for U-235m produced by Nuclear Excitation by Electronic Transition
NASA Astrophysics Data System (ADS)
Chodash, Perry; Norman, Eric; Burke, Jason; Wilks, Scott; Casperson, Robert
2014-09-01
Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that is predicted to occur in numerous isotopes, including U-235. When a nuclear transition matches the energy and the multipolarity of an electronic transition, there is a possibility that NEET will occur. If NEET were to occur in U-235, the nucleus would be excited to its 1/2 + isomeric state that subsequently decays by internal conversion with a decay energy of 77 eV and a half-life of 26 minutes. Theory predicts that NEET can occur in partially ionized uranium plasma with a charge state of 23 +. A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 780 mJ and a pulse width of 9 ns was used to generate the uranium plasma. The laser was focused on small samples of both depleted uranium and highly enriched uranium. The plasma conditions created by the intense laser pulse were varied by changing the spot size of the laser on the target. The resulting plasma was collected on a plate and the internal conversion electrons were focused onto a microchannel plate detector by a series of electrostatic lenses. First results will be presented. Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that is predicted to occur in numerous isotopes, including U-235. When a nuclear transition matches the energy and the multipolarity of an electronic transition, there is a possibility that NEET will occur. If NEET were to occur in U-235, the nucleus would be excited to its 1/2 + isomeric state that subsequently decays by internal conversion with a decay energy of 77 eV and a half-life of 26 minutes. Theory predicts that NEET can occur in partially ionized uranium plasma with a charge state of 23 +. A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 780 mJ and a pulse width of 9 ns was used to generate the uranium plasma. The laser was focused on small samples of both depleted uranium and highly enriched uranium. The plasma conditions created by the intense laser pulse were varied by changing the spot size of the laser on the target. The resulting plasma was collected on a plate and the internal conversion electrons were focused onto a microchannel plate detector by a series of electrostatic lenses. First results will be presented. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. The U.S. DHS, UC Berkeley, the NNIS fellowship and the NSSC further supported this work.
(234)U/(238)U signatures associated with uranium ore bodies: part 3 Koongarra.
Lowson, Richard T
2013-04-01
The Koongarra ore body is an early Proterozoic U ore body in the Alligator Rivers U province, Northern Territory, Australia. It has surface expression with a redox front located ∼30 m below the surface. The (234)U/(238)U activity ratios (AR) for the ground water and the amorphous phase of the solid have been analysed for the ore zone and dispersion halo as a function of depth. The results display a (234)U/(238)U AR signature with depth which may be common to all U ore bodies. The (234)U/(238)U AR is depressed below secular equilibrium in the weathered material above the redox front; rises significantly above secular equilibrium in the vicinity of the redox front; and is followed by a gradual decrease with depth below the redox front. The amplitude of the profile is a function of local conditions. A model is proposed for the signature in which oxidising waters preferentially leach the (234)U sites at the redox front due to preconditioning of the (234)U sites by α recoil during the decay of (23)(8)U to (23)(4)U. Mass balance requires the solid material left behind the redox front to have a (234)U/(238)U AR reduced below 1. Local second order effects may be superimposed on the signature. The signature may have application to calibrating scenarios for nuclear waste repositories, assisting in understanding historical climates, economic evaluation of U ore bodies and U exploration. Copyright © 2012 Elsevier Ltd. All rights reserved.
Measurement of 238U and 232Th radionuclides in ilmenite and synthetic rutile
NASA Astrophysics Data System (ADS)
Idris, M. I.; Siong, K. K.; Fadzil, S. M.
2018-01-01
The only factory that currently processes ilmenite to produce synthetic rutile is Tor Minerals in Ipoh, Perak, Malaysia. These two minerals contain radioactive elements such as uranium and thorium. Furthermore, this factory was built close to the residential areas. Thus, the primary issues are radiation exposure attributed to the decay of the radionuclides. Hence, the objectives of this study are to measure the dose and to evaluate activity levels of uranium and thorium. Dose rates from surrounding area of factory indicate the normal range for both on the surface and 1 meter above the ground (0.3-0.7 μSv/hr) lower than the global range of 0.5-1.3 μSv/hr set by UNSCEAR. The mean activity levels of uranium and thorium for ilmenite are 235 Bq/kg and 503 Bq/kg while for synthetic rutile are 980 Bq/kg and 401 Bq/kg, respectively. The result shows that uranium activity levels of synthetic rutile is 4 times higher than ilmenite but it is still lower than the regulatory exemption limit of 1000 Bq/kg set by IAEA Basic Safety Standards. Even though the dose rates at the factory and the activity levels are within safe limits, safety precautions must be followed by the factory management to prevent any unwanted accident to occur.
Actinides in deer tissues at the rocky flats environmental technology site.
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.
Rapid cooling rates at an active mid-ocean ridge from zircon thermochronology
Schmitt, Axel K.; Perfit, Michael R.; Rubin, Kenneth H.; Stockli, Daniel F.; Smith, Matthew C.; Cotsonika, Laurie A.; Zellmer, Georg F.; Ridley, W. Ian
2011-01-01
Oceanic spreading ridges are Earth's most productive crust generating environment, but mechanisms and rates of crustal accretion and heat loss are debated. Existing observations on cooling rates are ambiguous regarding the prevalence of conductive vs. convective cooling of lower oceanic crust. Here, we report the discovery and dating of zircon in mid-ocean ridge dacite lavas that constrain magmatic differentiation and cooling rates at an active spreading center. Dacitic lavas erupted on the southern Cleft segment of the Juan de Fuca ridge, an intermediate-rate spreading center, near the intersection with the Blanco transform fault. Their U–Th zircon crystallization ages (29.3-4.6+4.8 ka; 1δ standard error s.e.) overlap with the (U–Th)/He zircon eruption age (32.7 ± 1.6 ka) within uncertainty. Based on similar 238U-230Th disequilibria between southern Cleft dacite glass separates and young mid-ocean ridge basalt (MORB) erupted nearby, differentiation must have occurred rapidly, within ~ 10–20 ka at most. Ti-in-zircon thermometry indicates crystallization at 850–900 °C and pressures > 70–150 MPa are calculated from H2O solubility models. These time-temperature constraints translate into a magma cooling rate of ~ 2 × 10-2 °C/a. This rate is at least one order-of-magnitude faster than those calculated for zircon-bearing plutonic rocks from slow spreading ridges. Such short intervals for differentiation and cooling can only be resolved through uranium-series (238U–230Th) decay in young lavas, and are best explained by dissipating heat convectively at high crustal permeability.
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
Uranium series, volcanic rocks
Vazquez, Jorge A.
2014-01-01
Application of U-series dating to volcanic rocks provides unique and valuable information about the absolute timing of crystallization and differentiation of magmas prior to eruption. The 238U–230Th and 230Th-226Ra methods are the most commonly employed for dating the crystallization of mafic to silicic magmas that erupt at volcanoes. Dates derived from the U–Th and Ra–Th methods reflect crystallization because diffusion of these elements at magmatic temperatures is sluggish (Cherniak 2010) and diffusive re-equilibration is insignificant over the timescales (less than or equal to 10^5 years) typically associated with pre-eruptive storage of nearly all magma compositions (Cooper and Reid 2008). Other dating methods based on elements that diffuse rapidly at magmatic temperatures, such as the 40Ar/39Ar and (U–Th)/He methods, yield dates for the cooling of magma at the time of eruption. Disequilibrium of some short-lived daughters of the uranium series such as 210Po may be fractionated by saturation of a volatile phase and can be employed to date magmatic gas loss that is synchronous with volcanic eruption (e.g., Rubin et al. 1994).
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.
NASA Astrophysics Data System (ADS)
Purushothaman, S.; Reiter, M. P.; Haettner, E.; Dendooven, P.; Dickel, T.; Geissel, H.; Ebert, J.; Jesch, C.; Plass, W. R.; Ranjan, M.; Weick, H.; Amjad, F.; Ayet, S.; Diwisch, M.; Estrade, A.; Farinon, F.; Greiner, F.; Kalantar-Nayestanaki, N.; Knöbel, R.; Kurcewicz, J.; Lang, J.; Moore, I. D.; Mukha, I.; Nociforo, C.; Petrick, M.; Pfützner, M.; Pietri, S.; Prochazka, A.; Rink, A.-K.; Rinta-Antila, S.; Scheidenberger, C.; Takechi, M.; Tanaka, Y. K.; Winfield, J. S.; Yavor, M. I.
2013-11-01
A cryogenic stopping cell (CSC) has been commissioned with 238U projectile fragments produced at 1000 MeV/u. The spatial isotopic separation in flight was performed with the FRS applying a monoenergetic degrader. For the first time, a stopping cell was operated with exotic nuclei at cryogenic temperatures (70 to 100 K). A helium stopping gas density of up to 0.05\\ \\text{mg/cm}^3 was used, about two times higher than reached before for a stopping cell with RF ion repelling structures. An overall efficiency of up to 15%, a combined ion survival and extraction efficiency of about 50%, and extraction times of 24 ms were achieved for heavy α-decaying uranium fragments. Mass spectrometry with a multiple-reflection time-of-flight mass spectrometer has demonstrated the excellent cleanliness of the CSC. This setup has opened a new field for the spectroscopy of short-lived nuclei.
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.
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
Marine Chemistry in the People’s Republic of China.
1984-08-01
Eh, Fe, Al, Mn, Cu, Pb, Zn, Cd, Hg, Cr, and also the sedimentation rate by Pb- 210 method. (2) The effects of flow rate, eddy diffusion, axial length of...sediments, distribution, determination, radium-226, uranium-238, radon-222, polonium - 210 , bismuth- 210 , lead-206, particulates, adsorption, polonium ...sediments, distribution, radium-226, uranium-238, radon-222, polonium - 210 , bismuth- 210 , lead-206, particulates, adsorption, polonium , dating, Zhujiang
Fractal and Chaos Analysis for Dynamics of Radon Exhalation from Uranium Mill Tailings
NASA Astrophysics Data System (ADS)
Li, Yongmei; Tan, Wanyu; Tan, Kaixuan; Liu, Zehua; Xie, Yanshi
2016-08-01
Tailings from mining and milling of uranium ores potentially are large volumes of low-level radioactive materials. A typical environmental problem associated with uranium tailings is radon exhalation, which can significantly pose risks to environment and human health. In order to reduce these risks, it is essential to study the dynamical nature and underlying mechanism of radon exhalation from uranium mill tailings. This motivates the conduction of this study, which is based on the fractal and chaotic methods (e.g. calculating the Hurst exponent, Lyapunov exponent and correlation dimension) and laboratory experiments of the radon exhalation rates. The experimental results show that the radon exhalation rate from uranium mill tailings is highly oscillated. In addition, the nonlinear analyses of the time series of radon exhalation rate demonstrate the following points: (1) the value of Hurst exponent much larger than 0.5 indicates non-random behavior of the radon time series; (2) the positive Lyapunov exponent and non-integer correlation dimension of the time series imply that the radon exhalation from uranium tailings is a chaotic dynamical process; (3) the required minimum number of variables should be five to describe the time evolution of radon exhalation. Therefore, it can be concluded that the internal factors, including heterogeneous distribution of radium, and randomness of radium decay, as well as the fractal characteristics of the tailings, can result in the chaotic evolution of radon exhalation from the tailings.
The uranium-isotopic composition of Saharan dust collected over the central Atlantic Ocean
NASA Astrophysics Data System (ADS)
Aciego, Sarah M.; Aarons, Sarah M.; Sims, Kenneth W. W.
2015-06-01
Uranium isotopic compositions, (234U/238U)activity , are utilized by earth surface disciplines as chronometers and source tracers, including in soil science where aeolian dust is a significant source to the total nutrient pool. However, the (234U/238U)activity composition of dust is under characterized due to material and analytical constraints. Here we present new uranium isotope data measured by high precision MC-ICP-MS on ten airborne dust samples collected on the M55 trans-Atlantic cruise in 2002. Two pairs of samples are presented with different size fractions, coarse (1-30 μm) and fine (<1 μm), and all samples were processed to separate the water soluble component in order to assess the controls on the (234U/238U)activity of mineral aerosols transported from the Sahara across the Atlantic. Our results indicate (234U/238U)activity above one for both the water soluble (1.13-1.17) and the residual solid (1.06-1.18) fractions of the dust; no significant correlation is found between isotopic composition and travel distance. Residual solids indicate a slight dependance of (234U/238U)activity on particle size. Future modeling work that incorporates dust isotopic compositions into mixing or isotopic fractionation models will need to account for the wide variability in dust (234U/238U)activity .
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.
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.
NASA Astrophysics Data System (ADS)
Cannon, B. D.
1993-10-01
Isotopically-selective excitation of uranium atoms by diode lasers can be the basis for a portable instrument to perform uranium isotopic assays in the field. Such an instrument would improve the ability of on-site inspections to detect and deter nuclear proliferation. Published and unpublished spectroscopic data on atomic uranium were examined to identify candidate transitions for isotopically-selective laser excitation with diode lasers. Eleven candidate transitions were identified and evaluated for their potential usefulness for a portable uranium assay instrument. Eight of these transitions are suitable for laser induced fluorescence using different excitation and detection wavelengths, which will improve sensitivity and elemental selectivity. Data sheets on the 25 uranium transitions in the wavelength range 629 nm to 1,000 nm that originate in the ground or first excited states of neutral atomic uranium are included. Each data sheet provides the wavelength, upper and lower energy levels, angular momentum quantum numbers, U-235 isotope shift (relative to U-238, and high-resolution spectra of weapons-grade uranium (93% U-235 and 7% U-238).
Radon (222Rn) in ground water of fractured rocks: A diffusion/ion exchange model
Wood, W.W.; Kraemer, T.F.; Shapiro, A.
2004-01-01
Ground waters from fractured igneous and high-grade sialic metamorphic rocks frequently have elevated activity of dissolved radon (222Rn). A chemically based model is proposed whereby radium (226Ra) from the decay of uranium (238U) diffuses through the primary porosity of the rock to the water-transmitting fracture where it is sorbed on weathering products. Sorption of 226Ra on the fracture surface maintains an activity gradient in the rock matrix, ensuring a continuous supply of 226Ra to fracture surfaces. As a result of the relatively long half-life of 226Ra (1601 years), significant activity can accumulate on fracture surfaces. The proximity of this sorbed 226Ra to the active ground water flow system allows its decay progeny 222Rn to enter directly into the water. Laboratory analyses of primary porosity and diffusion coefficients of the rock matrix, radon emanation, and ion exchange at fracture surfaces are consistent with the requirements of a diffusion/ion- exchange model. A dipole-brine injection/withdrawal experiment conducted between bedrock boreholes in the high-grade metamorphic and granite rocks at the Hubbard Brook Experimental Forest, Grafton County, New Hampshire, United States (42??56???N, 71??43???W) shows a large activity of 226Ra exchanged from fracture surfaces by a magnesium brine. The 226Ra activity removed by the exchange process is 34 times greater than that of 238U activity. These observations are consistent with the diffusion/ion-exchange model. Elutriate isotopic ratios of 223Ra/226Ra and 238U/226Ra are also consistent with the proposed chemically based diffusion/ion-exchange model.
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.
NASA Astrophysics Data System (ADS)
Vengosh, A.; Pery, N.; Paytan, A.; Haquin, G.; Elhanani, S.; Pankratov, I.
2006-05-01
Many aquifer systems are composed of multiple rock types. Previous attempts to evaluate the specific aquifer rocks that control the groundwater chemistry and possible flow paths within these multiple lithological systems have used major ion chemistry and isotopic tracers (e.g., strontium isotopes). Here we propose an additional isotopic proxy that is based on the distribution of radium isotopes in groundwater. Radium has four radioactive isotopes that are part of the decay chains of uranium-238, thorium-232, and uranium-235. The abundance of radium isotope quartet (226Ra-half life 1600 y; 228Ra-5.6 y; 224Ra-3.6 d; 223Ra-11.4 d) in groundwater reflects the Th/U ratios in the rocks. Investigation of groundwater from the Negev, Israel, enabled us to discriminate between groundwaters flowing in the Lower Cretaceous Nubian Sandstone and the Upper Cretaceous Judea Group carbonate aquifers. Groundwater flowing in the sandstone aquifer has distinguishably high 228Ra/226Ra and 224Ra/223Ra ratios due to the high Th/U ratio in sandstone. In contrast, the predominance of uranium in carbonate rocks results in low 228Ra/226Ra and 224Ra/223Ra ratios in the associated groundwater. We show that the radium activity in groundwater in the two-aquifer systems is correlated with temperature, dissolved oxygen, and salinity. The increase of radium activity is also associated with changes in the isotopic ratios; 228Ra/226Ra ratios increase and decrease in the sandstone and carbonate aquifers, respectively. Given that the dissolution of radium isotopes depends on their decay constants, the use of the four radium isotopes with different decay constants enabled us to distinguish between dissolution (higher abundance of the long-lived isotopes) and recoil (predominance of the short-lived isotopes) processes. In spite of these isotopic fractionations, the radium isotopic discrimination between carbonate and sandstone aquifers is significant.
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.
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.
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.
Seltzer, Michael D
2003-09-01
Laser ablation of pressed soil pellets was examined as a means of direct sample introduction to enable inductively coupled plasma mass spectrometry (ICP-MS) screening of soils for residual depleted uranium (DU) contamination. Differentiation between depleted uranium, an anthropogenic contaminant, and naturally occurring uranium was accomplished on the basis of measured 235U/238U isotope ratios. The amount of sample preparation required for laser ablation is considerably less than that typically required for aqueous sample introduction. The amount of hazardous laboratory waste generated is diminished accordingly. During the present investigation, 235U/238U isotope ratios measured for field samples were in good agreement with those derived from gamma spectrometry measurements. However, substantial compensation was required to mitigate the effects of impaired pulse counting attributed to sample inhomogeneity and sporadic introduction of uranium analyte into the plasma.
CHEMICAL DIFFERENCES BETWEEN SLUDGE SOLIDS AT THE F AND H AREA TANK FARMS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Reboul, S.
2012-08-29
The primary source of waste solids received into the F Area Tank Farm (FTF) was from PUREX processing performed to recover uranium and plutonium from irradiated depleted uranium targets. In contrast, two primary sources of waste solids were received into the H Area Tank Farm (HTF): a) waste from PUREX processing; and b) waste from H-modified (HM) processing performed to recover uranium and neptunium from burned enriched uranium fuel. Due to the differences between the irradiated depleted uranium targets and the burned enriched uranium fuel, the average compositions of the F and H Area wastes are markedly different from onemore » another. Both F and H Area wastes contain significant amounts of iron and aluminum compounds. However, because the iron content of PUREX waste is higher than that of HM waste, and the aluminum content of PUREX waste is lower than that of HM waste, the iron to aluminum ratios of typical FTF waste solids are appreciably higher than those of typical HTF waste solids. Other constituents present at significantly higher concentrations in the typical FTF waste solids include uranium, nickel, ruthenium, zinc, silver, cobalt and copper. In contrast, constituents present at significantly higher concentrations in the typical HTF waste solids include mercury, thorium, oxalate, and radionuclides U-233, U-234, U-235, U-236, Pu-238, Pu-242, Cm-244, and Cm-245. Because of the higher concentrations of Pu-238 in HTF, the long-term concentrations of Th-230 and Ra-226 (from Pu-238 decay) will also be higher in HTF. The uranium and plutonium distributions of the average FTF waste were found to be consistent with depleted uranium and weapons grade plutonium, respectively (U-235 comprised 0.3 wt% of the FTF uranium, and Pu-240 comprised 6 wt% of the FTF plutonium). In contrast, at HTF, U-235 comprised 5 wt% of the uranium, and Pu-240 comprised 17 wt% of the plutonium, consistent with enriched uranium and high burn-up plutonium. X-ray diffraction analyses of various FTF and HTF samples indicated that the primary crystalline compounds of iron in sludge solids are Fe{sub 2}O{sub 3}, Fe{sub 3}O{sub 4}, and FeO(OH), and the primary crystalline compounds of aluminum are Al(OH){sub 3} and AlO(OH). Also identified were carbonate compounds of calcium, magnesium, and sodium; a nitrated sodium aluminosilicate; and various uranium compounds. Consistent with expectations, oxalate compounds were identified in solids associated with oxalic acid cleaning operations. The most likely oxidation states and chemical forms of technetium are assessed in the context of solubility, since technetium-99 is a key risk driver from an environmental fate and transport perspective. The primary oxidation state of technetium in SRS sludge solids is expected to be Tc(IV). In salt waste, the primary oxidation state is expected to be Tc(VII). The primary form of technetium in sludge is expected to be a hydrated technetium dioxide, TcO{sub 2} {center_dot} xH{sub 2}O, which is relatively insoluble and likely co-precipitated with iron. In salt waste solutions, the primary form of technetium is expected to be the very soluble pertechnetate anion, TcO{sub 4}{sup -}. The relative differences between the F and H Tank Farm waste provide a basis for anticipating differences that will occur as constituents of FTF and HTF waste residue enter the environment over the long-term future. If a constituent is significantly more dominant in one of the Tank Farms, its long-term environmental contribution will likely be commensurately higher, assuming the environmental transport conditions of the two Tank Farms share some commonality. It is in this vein that the information cited in this document is provided - for use during the generation, assessment, and validation of Performance Assessment modeling results.« less
The chronology for the d18O record from Devils Hole, Nevada, extended into the Mid-Holocene
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.
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).
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.
Sheen, Seungsoo; Lee, Keu Sung; Chung, Wou Young; Nam, Saeil; Kang, Dae Ryong
2016-01-01
Lung cancer is a leading cause of cancer-related death in the world. Smoking is definitely the most important risk factor for lung cancer. Radon ((222)Rn) is a natural gas produced from radium ((226)Ra) in the decay series of uranium ((238)U). Radon exposure is the second most common cause of lung cancer and the first risk factor for lung cancer in never-smokers. Case-control studies have provided epidemiological evidence of the causative relationship between indoor radon exposure and lung cancer. Twenty-four case-control study papers were found by our search strategy from the PubMed database. Among them, seven studies showed that indoor radon has a statistically significant association with lung cancer. The studies performed in radon-prone areas showed a more positive association between radon and lung cancer. Reviewed papers had inconsistent results on the dose-response relationship between indoor radon and lung cancer risk. Further refined case-control studies will be required to evaluate the relationship between radon and lung cancer. Sufficient study sample size, proper interview methods, valid and precise indoor radon measurement, wide range of indoor radon, and appropriate control of confounders such as smoking status should be considered in further case-control studies.
234U/238U as a ground-water tracer, SW Nevada-SE California
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.
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.
Search for Nuclear Excitation by Electronic Transition in U-235
NASA Astrophysics Data System (ADS)
Chodash, P. A.; Norman, E. B.; Burke, J. T.; Wilks, S. C.; Casperson, R. J.; Swanberg, E. L.; Wakeling, M. A.; Cordeiro, T. J.
2013-10-01
Nuclear excitation by electronic transition (NEET) is a rare nuclear excitation that is predicted to occur in numerous isotopes, including U-235. When a nuclear transition matches the energy and the multipolarity of an electronic transition, there is a possibility that NEET will occur. If NEET were to occur in U-235, the nucleus would be excited to its 1/2 + isomeric state that subsequently decays by internal conversion with a decay energy of 77 eV and a half-life of 26 minutes. Theory predicts that NEET can occur in partially ionized uranium plasma with a charge state of 23 +. A pulsed Nd:YAG laser operating at 1064 nm with a pulse energy of 780 mJ and a pulse width of 9 ns was used to generate the uranium plasma. The plasma was collected on a plate and the internal conversion electrons were focused onto a microchannel plate detector by a series of electrostatic lenses. Depleted uranium and highly enriched uranium samples were used for the experiment. Preliminary results will be presented. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under contract DE-AC52-07NA27344. This work was further supported by the U.S. DHS, UC Berkeley, and the NNIS Fellowship.
Measurement of radioactive contamination in the CCD’s of the DAMIC experiment
NASA Astrophysics Data System (ADS)
Aguilar-Arevalo, A.; Amidei, D.; Bertou, X.; Bole, D.; Butner, M.; Cancelo, G.; Castañeda Vásquez, A.; Chavarria, A. E.; de Mello Neto, J. R. T.; Dixon, S.; D'Olivo, J. C.; Estrada, J.; Fernandez Moroni, G.; Hernández Torres, K. P.; Izraelevitch, F.; Kavner, A.; Kilminster, B.; Lawson, I.; Liao, J.; López, M.; Molina, J.; Moreno-Granados, G.; Pena, J.; Privitera, P.; Sarkis, Y.; Scarpine, V.; Schwarz, T.; Sofo Haro, M.; Tiffenberg, J.; Torres Machado, D.; Trillaud, F.; Yol, X.; Zhou, J.
2016-05-01
DAMIC (Dark Matter in CCDs) is an experiment searching for dark matter particles employing fully-depleted charge-coupled devices. Using the bulk silicon which composes the detector as target, we expect to observe coherent WIMP-nucleus elastic scattering. Although located in the SNOLAB laboratory, 2 km below the surface, the CCDs are not completely free of radioactive contamination, in particular coming from radon daughters or from the detector itself. We present novel techniques for the measurement of the radioactive contamination in the bulk silicon and on the surface of DAMIC CCDs. Limits on the Uranium and Thorium contamination as well as on the cosmogenic isotope 32 Si, intrinsically present on the detector, were performed. We have obtained upper limits on the 238 TJ (232 Th) decay rate of 5 (15) kg_1 d_1 at 95% CL. Pairs of spatially correlated electron tracks expected from 32 Si-32 P and 210 Pb-210 Bi beta decays were also measured. We have found a decay rate of 80+l10 -65 kg_1 d_1 for 32 Si and an upper limit of - 35 kg-1 d-1 for 210 Pb, both at 95% CL.
Radium and uranium levels in vegetables grown using different farming management systems.
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.
NASA Astrophysics Data System (ADS)
Gillmore, G.; Woods, M.
2009-04-01
Radon isotopes (222, 220, 219) are radioactive gases produced by the disintegration of radium isotopes 226, 224 and 223, which are decay products of uranium238, thorium232 and uranium235 respectively. All are found in the earth's crust. Solid elements, also radioactive, are produced by radon disintegration. Radon is classed as a rare gas in the periodic table of elements, along with helium, argon, neon, krypton and xenon. When disintegrating, radon emits alpha particles and generates solid decay products, which are also radioactive (polonium, bismuth, lead etc.). The potential danger of radon lies in its solid decay products rather than the gas itself. Whether or not they are attached aerosols, radon decay products can be inhaled and deposited in the bronchopulmonary tree to varying depths according to their size. Radon today is considered to be the main source of human exposure to natural radiation. At the international level, radon accounts for 52% of global average exposure to natural radiation. Isotope 222 (48%) is far more significant than isotope 220 (4%), whilst isotope 219 is considered as negligible. Exposure to radon varies considerably from one region to another, depending on factors such as weather conditions, and underlying geology. Activity concentration can therefore vary by a factor of 10 or even a 100 from one period of time to the next and from one area to another. There are many ways of measuring the radon 222 activity concentration and the potential alpha energy concentration of its short-lived decay products. Measuring techniques fall into three categories: - spot measurement methods; continuous measurement; integrated measurement. The proposed ISO (International Organisation for Standardisation) document suggests guidelines for measuring radon222 activity concentration and the potential alpha energy concentration of its short-lived decay products in a free (environment) and confined (buildings) atmosphere. The target date for availability of this work item is 2011. The ISO document here highlighted is a working draft. ISO is a worldwide federation of national standards bodies. Keywords: radon; international standards; measurement techniques.
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].
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%.
NASA Astrophysics Data System (ADS)
Tissot, François L. H.; Dauphas, Nicolas
2015-10-01
The 238U/235U isotopic composition of uranium in seawater can provide important insights into the modern U budget of the oceans. Using the double spike technique and a new data reduction method, we analyzed an array of seawater samples and 41 geostandards covering a broad range of geological settings relevant to low and high temperature geochemistry. Analyses of 18 seawater samples from geographically diverse sites from the Atlantic and Pacific oceans, Mediterranean Sea, Gulf of Mexico, Persian Gulf, and English Channel, together with literature data (n = 17), yield a δ238U value for modern seawater of -0.392 ± 0.005‰ relative to CRM-112a. Measurements of the uranium isotopic compositions of river water, lake water, evaporites, modern coral, shales, and various igneous rocks (n = 64), together with compilations of literature data (n = 380), allow us to estimate the uranium isotopic compositions of the various reservoirs involved in the modern oceanic uranium budget, as well as the fractionation factors associated with U incorporation into those reservoirs. Because the incorporation of U into anoxic/euxinic sediments is accompanied by large isotopic fractionation (ΔAnoxic/Euxinic-SW = +0.6‰), the size of the anoxic/euxinic sink strongly influences the δ238U value of seawater. Keeping all other fluxes constant, the flux of uranium in the anoxic/euxinic sink is constrained to be 7.0 ± 3.1 Mmol/yr (or 14 ± 3% of the total flux out of the ocean). This translates into an areal extent of anoxia into the modern ocean of 0.21 ± 0.09% of the total seafloor. This agrees with independent estimates and rules out a recent uranium budget estimate by Henderson and Anderson (2003). Using the mass fractions and isotopic compositions of various rock types in Earth's crust, we further calculate an average δ238U isotopic composition for the continental crust of -0.29 ± 0.03‰ corresponding to a 238U/235U isotopic ratio of 137.797 ± 0.005. We discuss the implications of the variability of the 238U/235U ratio on Pb-Pb and U-Pb ages and provide analytical formulas to calculate age corrections as a function of the age and isotopic composition of the sample. The crustal ratio may be used in calculation of Pb-Pb and U-Pb ages of continental crust rocks and minerals when the U isotopic composition is unknown. In cosmochemistry, the search for 247Cm (t1/2 = 15.6 Myr), an extinct short-lived radionuclide that decays into 235U, is important for understanding how r-process nuclides were synthesized in stars and learning about the astrophysical context of solar system formation (Chen and Wasserburg, 1981; Wasserburg et al., 1996; Nittler and Dauphas, 2006; Brennecka et al., 2010b; Tissot et al., 2015). In both terrestrial and extraterrestrial samples, variations in the 238U/235U ratio affect Pb-Pb ages (and depending on the analytical protocols, U-Pb ages). Therefore, samples dated by these techniques need to have their U isotopic compositions measured (Stirling et al., 2005, 2006; Weyer et al., 2008; Amelin et al., 2010; Brennecka et al., 2010b; Brennecka and Wadhwa, 2012; Connelly et al., 2012; Goldmann et al., 2015) or uncertainties on the U isotopic composition should be propagated into age calculations. In low temperature aqueous geochemistry, U isotopic fractionation between U4+ and U6+ (driven in part by nuclear field shift effects; Bigeleisen, 1996; Schauble, 2007; Abe et al., 2008), makes U isotopes potential tracers of paleoredox conditions (Montoya-Pino et al., 2010; Brennecka et al., 2011a; Kendall et al., 2013, 2015; Asael et al., 2013; Andersen et al., 2014; Dahl et al., 2014; Goto et al., 2014; Noordmann et al., 2015). The present paper aims at constraining some aspects of the global budget of uranium in the modern oceans using 238U/235U isotope variations, which involves characterizing the U isotopic composition of seawater and several reservoirs involved in the uranium oceanic budget. Uranium can exist in two oxidation states in terrestrial surface environments: U4+ is insoluble in seawater while U6+ is soluble (Langmuir, 1978). The contrasting behaviors of the two oxidation states of uranium explains why the disappearance of detrital uraninite after the Archean marks the rise of oxygen in Earth's atmosphere/hydrosphere (Ramdohr, 1958; Rasmussen and Buick, 1999; Frimmel, 2005). More recently, significant effort has focused on using U isotopes to constrain the past extents of anoxic/euxinic vs. oxic or suboxic sediments in modern and ancient oceans (Montoya-Pino et al., 2010; Brennecka et al., 2011a; Asael et al., 2013; Kendall et al., 2013, 2015; Andersen et al., 2014; Dahl et al., 2014; Goto et al., 2014; Noordmann et al., 2015). A virtue of this system is that it can potentially reflect the global redox state of Earth's oceans. At the same time, several difficulties have been encountered in applying U isotopes as paleo-redox indicators. For example, detrital contributions can blur the authigenic signal and have to be corrected for (Asael et al., 2013; Andersen et al., 2014; Noordmann et al., 2015), uranium isotopes can be affected by diagenesis and exchange with porewater (Romaniello et al., 2013; Andersen et al., 2014), and the exact isotopic fractionation factors relevant to various conditions of deposition are uncertain. While significant progress has already been made to address these difficulties (Asael et al., 2013; Romaniello et al., 2013; Andersen et al., 2014; Noordmann et al., 2015), this system and others are missing some of the groundwork studies on modern environments that are needed to gain trust in their applications to ancient sediments.In the modern ocean, water-soluble uranium behaves conservatively (i.e., U concentration correlates linearly to water salinity, Ku et al., 1977; Owens et al., 2011) and has a long residence time of ∼400 kyr (Ku et al., 1977). The ocean is therefore a large repository of uranium, exceeding the total inventory of land-based deposits (Lu, 2014). The riverine input (40-46 Mmol/yr) is balanced by several sinks; including suboxic sediments, anoxic/euxinic sediments, carbonates, altered oceanic crust, salt marshes and Fe-Mn nodules. Barnes and Cochran (1990), Morford and Emerson (1999), Dunk et al. (2002), and Henderson and Anderson (2003) each proposed estimates for the oceanic uranium budget that differ substantially in the fluxes that they use. Uranium isotopes are sensitive to ocean redox conditions because uranium removal in anoxic/euxinic sediments imparts large uranium isotopic fractionation, so that the areal extent of this sink influences greatly the U isotopic composition of seawater relative to the riverine input. In the present paper, we report double-spike uranium isotopic measurements of 18 seawater samples, 18 continental crust lithologies, 7 individual minerals, 6 oyster samples, 3 modern evaporites samples, 2 lake water samples, 1 large river water sample and 1 coral sample. These measurements are supplemented by compilations of literature data. With this large data set (n = 444), we are able to constrain the flux of uranium into anoxic/euxinic sediments, as well as the global extent of anoxia in the modern ocean (percent of seafloor covered by anoxic/euxinic sediments). Our findings compare well with independent estimates and rule out the most recent U budget of Henderson and Anderson (2003).As part of our effort, we also present a data reduction method for double-spike measurements that is both comprehensive in the way the errors are propagated and simple to implement.
Controlling Pu behavior on Titania: Implications for LEU Fission-Based Mo-99 Production
DOE Office of Scientific and Technical Information (OSTI.GOV)
Youker, Amanda J.; Brown, M. Alex; Heltemes, Thad A.
Molybdenum-99 is the parent isotope of the most widely used isotope, technetium-99m, in all diagnostic nuclear medicine procedures. Due to proliferation concerns associated with the use of highly enriched uranium (HEU), the preferred method of fission-based Mo-99 production uses low enriched uranium (LEU) targets. Using LEU versus HEU for Mo-99 production produces similar to 30 times more Pu-239, due to neutron capture on U-238 to produce Np-239, which ultimately decays to Pu-239 (t(1/2) = 24,110 yr). Argonne National Laboratory is supporting a potential US Mo-99 producer in their efforts to produce Mo-99 from an LEU solution. In order to mitigatemore » the generation of large volumes of greater-than-class-C (GTCC) low level waste (Pu-239 concentrations greater than 1 nCi/g), we have focused our efforts on the separation chemistry of Pu and Mo with a titania sorbent in sulfate media. Results from batch and column experiments show that temperature and acid wash concentration can be used to control Pu behavior on titania.« less
Pérez-Fernández, María A; Vera-Tomé, Feliciano; Blanco-Rodríguez, María P; Lozano, Juan C
2014-06-01
The evolution of vegetation structure following mine rehabilitation is rather scarce in the literature. The concentration of long-lived radionuclides of the (238)U series might have harmful effects on living organisms. We studied soil properties and the natural vegetation occurring along a gradient in Los Ratones, an area rehabilitated after uranium mining located in Cáceres, Spain. Soil and vegetation were sampled seasonally and physical and chemical properties of soil were analysed, including natural isotopes of (238)U, (230)Th, (226)Ra and (210)Pb. Species richness, diversity, evenness and plant cover were estimated and correlated in relation to soil physical and chemical variables. The location of the sampling sites along a gradient had a strong explanatory effect on the herbaceous species, as well as the presence of shrubs and trees. Seasonal effects of the four natural isotopes were observed in species richness, species diversity and plant cover; these effects were directly related to the pH values in the soil, this being the soil property that most influences the plant distribution. Vegetation in the studied area resembles that of the surroundings, thus proving that the rehabilitation carried out in Los Ratones mine was successful in terms of understorey cover recovery.
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.
Lyons, P.C.; Krogh, T.E.; Kwok, Y.Y.; Davis, D.W.; Outerbridge, W.F.; Evans, H.T.
2006-01-01
The Fire Clay tonstein [Pennsylvanian (Upper Carboniferous), Westphalian Series, Duckmantian Stage]-a kaolinized, volcanic-ash deposit occurring in Kentucky, West Virginia, Tennessee, and Virginia-is the most widespread bed in the Middle Pennsylvanian of the central Appalachian basin, USA. A concordant single-crystal U-Pb zircon datum for this tonstein gives a 206Pb/238U age of 314.6 ?? 0.9 Ma (2??). This age is in approximate agreement with a mean sanidine plateau age of 311.5 ?? 1.3 Ma (1??, n = 11) for the Fire Clay tonstein. The difference between the two ages may be due to bias between the 40K and 238U decay constants and other factors. The age of the Fire Clay tonstein has important implications for Duckmantian Stage (Westphalian Series) sedimentation rates, correlations with the Westphalian Series of Europe, Middle Pennsylvanian volcanic events, and the late Paleozoic time scale. ?? 2006 Elsevier B.V. All rights reserved.
Xing, Shan; Zhang, Weichao; Qiao, Jixin; Hou, Xiaolin
2018-09-01
In order to measure trace plutonium and its isotopes ratio ( 240 Pu/ 239 Pu) in environmental samples with a high uranium, an analytical method was developed using radiochemical separation for separation of plutonium from matrix and interfering elements including most of uranium and ICP-MS for measurement of plutonium isotopes. A novel measurement method was established for extensively removing the isobaric interference from uranium ( 238 U 1 H and 238 UH 2 + ) and tailing of 238 U, but significantly improving the measurement sensitivity of plutonium isotopes by employing NH 3 /He as collision/reaction cell gases and MS/MS system in the triple quadrupole ICP-MS instrument. The results show that removal efficiency of uranium interference was improved by more than 15 times, and the sensitivity of plutonium isotopes was increased by a factor of more than 3 compared to the conventional ICP-MS. The mechanism on the effective suppress of 238 U interference for 239 Pu measurement using NH 3 -He reaction gases was explored to be the formation of UNH + and UNH 2 + in the reactions of UH + and U + with NH 3 , while no reaction between NH 3 and Pu + . The detection limits of this method were estimated to be 0.55 fg mL -1 for 239 Pu, 0.09 fg mL -1 for 240 Pu. The analytical precision and accuracy of the method for Pu isotopes concentration and 240 Pu/ 239 Pu atomic ratio were evaluated by analysis of sediment reference materials (IAEA-385 and IAEA-412) with different levels of plutonium and uranium. The developed method were successfully applied to determine 239 Pu and 240 Pu concentrations and 240 Pu/ 239 Pu atomic ratios in soil samples collected in coastal areas of eastern China. Copyright © 2018 Elsevier B.V. All rights reserved.
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.
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.
Alpha-emitting isotopes and chromium in a coastal California aquifer
Densmore, Jill N.; Izbicki, John A.; Murtaugh, Joseph M.; Swarzenski, Peter W.; Bullen, Thomas D.
2014-01-01
The unadjusted 72-h gross alpha activities in water from two wells completed in marine and alluvial deposits in a coastal southern California aquifer 40 km north of San Diego were 15 and 25 picoCuries per liter (pCi/L). Although activities were below the Maximum Contaminant Level (MCL) of 15 pCi/L, when adjusted for uranium activity; there is concern that new wells in the area may exceed MCLs, or that future regulations may limit water use from the wells. Coupled well-bore flow and depth-dependent water-quality data collected from the wells in 2011 (with analyses for isotopes within the uranium, actinium, and thorium decay-chains) show gross alpha activity in marine deposits is associated with decay of naturally-occurring 238U and its daughter 234U. Radon activities in marine deposits were as high as 2230 pCi/L. In contrast, gross alpha activities in overlying alluvium within the Piedra de Lumbre watershed, eroded from the nearby San Onofre Hills, were associated with decay of 232Th, including its daughter 224Ra. Radon activities in alluvium from Piedra de Lumbre of 450 pCi/L were lower than in marine deposits. Chromium VI concentrations in marine deposits were less than the California MCL of 10 μg/L (effective July 1, 2014) but δ53Cr compositions were near zero and within reported ranges for anthropogenic chromium. Alluvial deposits from the nearby Las Flores watershed, which drains a larger area having diverse geology, has low alpha activities and chromium as a result of geologic and geochemical conditions and may be more promising for future water-supply development.
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.
Bartholomay, Roy C.; L. Flint Hall,
2016-05-05
The upper limit of background concentrations for radiochemical constituents for eastern regional water was 5.43 ±0.574 pCi/L for tritium, 0.0002048 ±0.0000054 pCi/L for chlorine-36, 0.000000865 ±0.000000015 pCi/L for iodine-129, <0.0000054 pCi/L for technetium-99, 0 pCi/L for strontium-90, plutonium-238, plutonium-239, -240 (undivided), and americium-241, 1.32 ±0.77 pCi/L for uranium-234, 0.016 ±0.012 pCi/L for uranium-235, and 0.477 ±0.044 pCi/L for uranium-238.
Investigation of the radiological impact on the coastal environment surrounding a fertilizer plant.
El Samad, O; Aoun, M; Nsouli, B; Khalaf, G; Hamze, M
2014-07-01
This investigation was carried out in order to assess the marine environmental radioactive pollution and the radiological impact caused by a large production plant of phosphate fertilizer, located in the Lebanese coastal zone. Natural radionuclides ((238)U, (235)U, (232)Th, (226)Ra, (210)Po, (210)Pb, (40)K) and anthropogenic (137)Cs were measured by alpha and gamma spectrometry in seawater, sediment, biota and coastal soil samples collected from the area impacted by this industry. The limited environmental monitoring program within 2 km of the plant indicates localized contamination with radionuclides of the uranium decay chain mainly due to the transport, the storage of raw materials and the free release of phosphogypsum waste. Copyright © 2013 Elsevier Ltd. All rights reserved.
The Effect of U-234 Content on the Neutronic Behavior of Uranium Systems
DOE Office of Scientific and Technical Information (OSTI.GOV)
Busch, Robert D.; Bledsoe, Keith C
2011-01-01
When analyzing uranium systems, the usual rule of thumb is to ignore the U-234 by assuming that it behaves neutronically like U-238. Thus for uranium systems, the uranium is evaluated as U-235 with everything else being U-238. The absorption cross section of U-234 is indeed qualitatively very similar to that of U-238. However, thermal absorption cross section of U-234 is about 100 times that of U-238. At low U-235 enrichments, the amount of U-234 is quite small so the impact of assuming it is U-238 is minimal. However, at high enrichments, the relative ratio of U-234 to U-238 is quitemore » large (maybe as much as 1 to 5). Thus, one would expect that some effect of using the rule of thumb might be seen in higher enriched systems. Analyses were performed on three uranium systems from the set of Benchmarks [1]. Although the benchmarks are adequately characterized as to the U-234 content, often, materials used in processing are not as well characterized. This issue may become more important with the advent of laser enrichment processes, which have little or no effect on the U-234 content. Analytical results based on the relationship of U-234 activity to that of U-235 have shown good predictive capability but with large variability in the uncertainties [2]. Rucker and Johnson noted that the actual isotopics vary with enrichment, design of the enrichment cascade, composition of the feed material, and on blending of enrichments so there is considerable uncertainty in the use of models to determine isotopics. Thus, it is important for criticality personnel to understand the effects of variation of U-234 content in fissile systems and the impact of different modeling assumptions in handling the U-234. Analyses were done on LEU, IEU and HEU benchmarks from the International Handbook. These indicate that the effect of ignoring U-234 in HEU metal systems is non-conservative while it seems to be conservative for HEU solution systems. The magnitude of change in k-effective was as high as 0.4%, which has implications on selection of administrative margins and the determination of the upper subcriticality limit.« less
Uranium in sediments, mussels (Mytilus sp.) and seawater of the Krka river estuary.
Cuculić, Vlado; Cukrov, Neven; Barisić, Delko; Mlakar, Marina
2006-01-01
The response of an aquatic environment to the decrease of phosphate discharges from a technologically improved transhipment terminal, situated at the Croatian Adriatic coast in the port of Sibenik, has been assessed based on uranium activity and concentration in sediment, seawater and mussels Mytilus sp. The highest 238U activities (485+/-16Bqkg(-1) dry weight) were found in the sediment sample collected from the sampling site closest to the terminal. The maximum concentrations in the sediment samples are above the natural ranges and clearly indicate the harbour activities' influence. The 238U/226Ra activity ratios in sediment samples demonstrate the decreasing trend of phosphate ore input. Mussel samples showed levels of 238U activities in the range from 12.1+/-2.9 to 19.4+/-7.2 Bqkg(-1) dry weight, thus being slightly higher than in normally consumed mussels. Only the seawater, taken just above the bottom sediment at the sampling site closest to the terminal, shows a slightly higher uranium concentration (3.1+/-0.2 microgL(-1)) when compared to the samples taken in upper seawater layers (2.1+/-0.2 microgL(-1)) but is in the range of the concentration level of uranium in natural seawater. Since the transhipment terminal in the port of Sibenik was modernised in 1988, discharge of phosphate ore into the seawater was drastically reduced and, consequently, uranium concentration levels in seawater have decreased. However, enhanced uranium activity levels are still found in deeper sediment layer samples and in mussel.
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
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.
MCNP modelling of scintillation-detector gamma-ray spectra from natural radionuclides.
Hendriks, P H G M; Maucec, M; de Meijer, R J
2002-09-01
gamma-ray spectra of natural radionuclides are simulated for a BGO detector in a borehole geometry using the Monte Carlo code MCNP. All gamma-ray emissions of the decay of 40K and the series of 232Th and 238U are used to describe the source. A procedure is proposed which excludes the time-consuming electron tracking in less relevant areas of the geometry. The simulated gamma-ray spectra are benchmarked against laboratory data.
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.
Van Gosen, Bradley S.; Hall, Susan M.
2017-12-18
This report describes the discovery and geology of two near-surface uranium deposits within calcareous lacustrine strata of Pleistocene age in west Texas, United States. Calcrete uranium deposits have not been previously reported in the United States. The west Texas uranium deposits share characteristics with some calcrete uranium deposits in Western Australia—uranium-vanadium minerals hosted by nonpedogenic calcretes deposited in saline lacustrine environments.In the mid-1970s, Kerr-McGee Corporation conducted a regional uranium exploration program in the Southern High Plains province of the United States, which led to the discovery of two shallow uranium deposits (that were not publicly reported). With extensive drilling, Kerr-McGee delineated one deposit of about 2.1 million metric tons of ore with an average grade of 0.037 percent U3O8 and another deposit of about 0.93 million metric tons of ore averaging 0.047 percent U3O8.The west-Texas calcrete uranium-vanadium deposits occur in calcareous, fine-grained sediments interpreted to be deposited in saline lakes formed during dry interglacial periods of the Pleistocene. The lakes were associated with drainages upstream of a large Pleistocene lake. Age determinations of tephra in strata adjacent to one deposit indicate the host strata is middle Pleistocene in age.Examination of the uranium-vanadium mineralization by scanning-electron microscopy indicated at least two generations of uranium-vanadium deposition in the lacustrine strata identified as carnotite and a strontium-uranium-vanadium mineral. Preliminary uranium-series results indicate a two-component system in the host calcrete, with early lacustrine carbonate that was deposited (or recrystallized) about 190 kilo-annum, followed much later by carnotite-rich crusts and strontium-uranium-vanadium mineralization in the Holocene (about 5 kilo-annum). Differences in initial 234U/238U activity ratios indicate two separate, distinct fluid sources.
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).
Mohammed, Najat K.; Mazunga, Mohamed S.
2013-01-01
The discovery of high concentration uranium deposit at Mkuju, southern part of Tanzania, has brought concern about the levels of natural radioactivity at villages in the neighborhood of the deposit. This study determined the radioactivity levels of 30 soil samples and 20 water samples from Likuyu village which is 54 km east of the uranium deposit. The concentrations of the natural radionuclides 238U, 232Th, and 40K were determined using low level gamma spectrometry of the Tanzania Atomic Energy Commission (TAEC) Laboratory in Arusha. The average radioactivity concentrations obtained in soil samples for 238U (51.7 Bq/kg), 232Th (36.4 Bq/kg), and 40K (564.3 Bq/kg) were higher than the worldwide average concentrations value of these radionuclides reported by UNSCEAR, 2000. The average activity concentration value of 238U (2.35 Bq/L) and 232Th (1.85 Bq/L) in water samples was similar and comparable to their mean concentrations in the control sample collected from Nduluma River in Arusha. PMID:23781247
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
NONE
1998-12-01
Accurate measurements of radioactivity in soils contaminated with Strontium-90 (Sr-90) or Uranium-238 (U-238) are essential for many DOE site remediation programs. These crucial measurements determine if excavation and soil removal is necessary, where remediation efforts should be focused, and/or if a site has reached closure. Measuring soil contamination by standard EPA laboratory methods typically takes a week (accelerated analytical test turnaround) or a month (standard analytical test turnaround). The time delay extends to operations involving heavy excavation equipment and associated personnel which are the main costs of remediation. This report describes an application of the BetaScint{trademark} fiber-optic sensor that measuresmore » Sr-90 or U-238 contamination in soil samples on site in about 20 minutes, at a much lower cost than time-consuming laboratory methods, to greatly facilitate remediation. This report describes the technology, its performance, its uses, cost, regulatory and policy issues, and lessons learned.« less
NASA Astrophysics Data System (ADS)
Nitzsche, O.; Merkel, B.
Knowledge of the transport behavior of radionuclides in groundwater is needed for both groundwater protection and remediation of abandoned uranium mines and milling sites. Dispersion, diffusion, mixing, recharge to the aquifer, and chemical interactions, as well as radioactive decay, should be taken into account to obtain reliable predictions on transport of primordial nuclides in groundwater. This paper demonstrates the need for carrying out rehabilitation strategies before closure of the Königstein in-situ leaching uranium mine near Dresden, Germany. Column experiments on drilling cores with uranium-enriched tap water provided data about the exchange behavior of uranium. Uranium breakthrough was observed after more than 20 pore volumes. This strong retardation is due to the exchange of positively charged uranium ions. The code TReAC is a 1-D, 2-D, and 3-D reactive transport code that was modified to take into account the radioactive decay of uranium and the most important daughter nuclides, and to include double-porosity flow. TReAC satisfactorily simulated the breakthrough curves of the column experiments and provided a first approximation of exchange parameters. Groundwater flow in the region of the Königstein mine was simulated using the FLOWPATH code. Reactive transport behavior was simulated with TReAC in one dimension along a 6000-m path line. Results show that uranium migration is relatively slow, but that due to decay of uranium, the concentration of radium along the flow path increases. Results are highly sensitive to the influence of double-porosity flow. Résumé La protection des eaux souterraines et la restauration des sites miniers et de prétraitement d'uranium abandonnés nécessitent de connaître le comportement des radionucléides au cours de leur transport dans les eaux souterraines. La dispersion, la diffusion, le mélange, la recharge de l'aquifère et les interactions chimiques, de même que la décroissance radioactive, doivent être prises en compte pour obtenir des prédictions fiables concernant le transport des nucléides primaires dans les eaux souterraines. Ce papier montre la nécessité d'établir des stratégies de réhabilitation avant la fermeture de la mine d'uranium de Knigstein, près de Dresde (Allemagne). Des expériences de lessivage en colonne sur des carottes avec de l'eau enrichie en uranium fournissent des données sur le comportement de l'échange de l'uranium. La restitution de l'uranium a été observée après un lessivage par un volume supérieur à 20 fois celui des pores. Ce fort retard est dûà l'échange d'ions uranium positifs. Le code TReAC est un code de transport réactif en 1D, 2D et 3D, qui a été modifié pour prendre en compte la décroissance radioactive de l'uranium et les principaux nucléides descendants, et pour introduire l'écoulement dans un milieu à double porosité. TReAC a simulé de façon satisfaisante les courbes de restitution des expériences sur colonne et a fourni une première approche des paramètres de l'échange. L'écoulement souterrain dans la région de la mine de Knigstein a été simulé au moyen du code FLOWPATH. Le comportement du transport réactif a été simulé avec TReAC en une dimension, le long d'un axe d'écoulement long de 6000 m. Les résultats montrent que la migration de l'uranium est relativement lente ; mais du fait de la décroissance radioactive de l'uranium, la concentration en radium le long de cet axe augmente. Les résultats sont très sensibles à l'influence de l'écoulement en milieu à double porosité.
NASA Technical Reports Server (NTRS)
Latourrette, T. Z.; Kennedy, A. K.; Wasserburg, G. J.
1993-01-01
Mid-ocean ridge basalts (MORBs) and ocean island basalts (OIBs) are derived by partial melting of the upper mantle and are marked by systematic excesses of thorium-230 activity relative to the activity of its parent, uranium-238. Experimental measurements of the distribution of thorium and uranium between the melt and solid residue show that, of the major phases in the upper mantle, only garnet will retain uranium over thorium. This sense of fractionation, which is opposite to that caused by clinopyroxene-melt partitioning, is consistent with the thorium-230 excesses observed in young oceanic basalts. Thus, both MORBs and OIBs must begin partial melting in the garnet stability field or below about 70 kilometers. A calculation shows that the thorium-230-uranium-238 disequilibrium in MORBs can be attributed to dynamic partial melting beginning at 80 kilometers with a melt porosity of 0.2 percent or more. This result requires that melting beneath ridges occurs in a wide region and that the magma rises to the surface at a velocity of at least 0.9 meter per year.
Radionuclides from past uranium mining in rivers of Portugal.
Carvalho, Fernando P; Oliveira, João M; Lopes, Irene; Batista, Aleluia
2007-01-01
During several decades and until a few years ago, uranium mines were exploited in the Centre of Portugal and wastewaters from uranium ore milling facilities were discharged into river basins. To investigate enhancement of radioactivity in freshwater ecosystems, radionuclides of uranium and thorium series were measured in water, sediments, suspended matter, and fish samples from the rivers Vouga, Dão, Távora and Mondego. The results show that these rivers carry sediments with relatively high naturally occurring radioactivity, and display relatively high concentrations of radon dissolved in water, which is typical of a uranium rich region. Riverbed sediments show enhanced concentrations of radionuclides in the mid-section of the Mondego River, a sign of past wastewater discharges from mining and milling works at Urgeiriça confirmed by the enhanced values of (238)U/(232)Th radionuclide ratios in sediments. Radionuclide concentrations in water, suspended matter and freshwater fish from that section of Mondego are also enhanced in comparison with concentrations measured in other rivers. Based on current radionuclide concentrations in fish, regular consumption of freshwater species by local populations would add 0.032 mSv a(-1) of dose equivalent (1%) to the average background radiation dose. Therefore, it is concluded that current levels of enhanced radioactivity do not pose a significant radiological risk either to aquatic fauna or to freshwater fish consumers.
Code of Federal Regulations, 2010 CFR
2010-01-01
.... Critical assembly means special nuclear devices designed and used to sustain nuclear reactions, which may... reaction becomes self-sustaining. Design features means the design features of a nuclear facility specified... reaction (e.g., uranium-233, uranium-235, plutonium-238, plutonium-239, plutonium-241, neptunium-237...
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.
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.
Radiation from plutonium 238 used in space applications
NASA Technical Reports Server (NTRS)
Keenan, T. K.; Vallee, R. E.; Powers, J. A.
1972-01-01
The principal mode of the nuclear decay of plutonium 238 is by alpha particle emission at a rate of 17 curies per gram. Gamma radiation also present in nuclear fuels arises primarily from the nuclear de-excitation of daughter nuclei as a result of the alpha decay of plutonium 238 and reactor-produced impurities. Plutonium 238 has a spontaneous fission half life of 4.8 x 10 to the 10th power years. Neutrons associated with this spontaneous fission are emitted at a rate of 28,000 neutrons per second per gram. Since the space fuel form of plutonium 238 is the oxide pressed into a cermet with molybdenum, a contribution to the neutron emission rate arises from (alpha, n) reactions with 0-17 and 0-18 which occur in natural oxygen.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Harold F. McFarlane; Terry Todd
2013-11-01
Reprocessing is essential to closing nuclear fuel cycle. Natural uranium contains only 0.7 percent 235U, the fissile (see glossary for technical terms) isotope that produces most of the fission energy in a nuclear power plant. Prior to being used in commercial nuclear fuel, uranium is typically enriched to 3–5% in 235U. If the enrichment process discards depleted uranium at 0.2 percent 235U, it takes more than seven tonnes of uranium feed to produce one tonne of 4%-enriched uranium. Nuclear fuel discharged at the end of its economic lifetime contains less one percent 235U, but still more than the natural ore.more » Less than one percent of the uranium that enters the fuel cycle is actually used in a single pass through the reactor. The other naturally occurring isotope, 238U, directly contributes in a minor way to power generation. However, its main role is to transmute into plutoniumby neutron capture and subsequent radioactive decay of unstable uraniumand neptuniumisotopes. 239Pu and 241Pu are fissile isotopes that produce more than 40% of the fission energy in commercially deployed reactors. It is recovery of the plutonium (and to a lesser extent the uranium) for use in recycled nuclear fuel that has been the primary focus of commercial reprocessing. Uraniumtargets irradiated in special purpose reactors are also reprocessed to obtain the fission product 99Mo, the parent isotope of technetium, which is widely used inmedical procedures. Among the fission products, recovery of such expensive metals as platinum and rhodium is technically achievable, but not economically viable in current market and regulatory conditions. During the past 60 years, many different techniques for reprocessing used nuclear fuel have been proposed and tested in the laboratory. However, commercial reprocessing has been implemented along a single line of aqueous solvent extraction technology called plutonium uranium reduction extraction process (PUREX). Similarly, hundreds of types of reactor fuels have been irradiated for different purposes, but the vast majority of commercial fuel is uranium oxide clad in zirconium alloy tubing. As a result, commercial reprocessing plants have relatively narrow technical requirements for used nuclear that is accepted for processing.« less
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.
Nuclear Propulsion for Space Applications
NASA Technical Reports Server (NTRS)
Houts, M. G.; Bechtel, R. D.; Borowski, S. K.; George, J. A.; Kim, T.; Emrich, W. J.; Hickman, R. R.; Broadway, J. W.; Gerrish, H. P.; Adams, R. B.
2013-01-01
Basics of Nuclear Systems: Long history of use on Apollo and space science missions. 44 RTGs and hundreds of RHUs launched by U.S. during past 4 decades. Heat produced from natural alpha (a) particle decay of Plutonium (Pu-238). Used for both thermal management and electricity production. Used terrestrially for over 65 years. Fissioning 1 kg of uranium yields as much energy as burning 2,700,000 kg of coal. One US space reactor (SNAP-10A) flown (1965). Former U.S.S.R. flew 33 space reactors. Heat produced from neutron-induced splitting of a nucleus (e.g. U-235). At steady-state, 1 of the 2 to 3 neutrons released in the reaction causes a subsequent fission in a "chain reaction" process. Heat converted to electricity, or used directly to heat a propellant. Fission is highly versatile with many applications.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hamzah, Zaini, E-mail: tengkuliana88@gmail.com; Rosli, Tengku Nurliana Tuan Mohd, E-mail: tengkuliana88@gmail.com; Saat, Ahmad, E-mail: tengkuliana88@gmail.com
An estuary is an area that has a free connection with the open sea and it is a dynamic semi-enclosed coastal bodies. Ex-mining, aquaculture and industrial areas in Selangor are the sources of pollutants discharged into the estuary water. Radionuclides are considered as pollutants to the estuary water. Gamma radiations emitted by natural radionuclides through their decaying process may give impact to human. The radiological effect of natural radionuclides which are {sup 226}Ra, {sup 228}Ra, {sup 40}K, {sup 238}U and {sup 232}Th, were explored by determining the respective activity concentrations in filtered water along the Langat estuary, Selangor. Meanwhile, in-more » situ water quality parameters such as temperature, dissolve oxygen (DO), salinity, total suspended solid (TSS), pH and turbidity were measured by using YSI portable multi probes meter. The activity concentration of {sup 226}Ra, {sup 228}Ra and {sup 40}K were determined by using gamma-ray spectrometry with high-purity germanium (HPGe) detector. The activity concentrations of {sup 226}Ra, {sup 228}Ra and {sup 40}K in samples are in the range of 0.17 - 0.67 Bq/L, 0.16 - 0.97 Bq/L and 1.22 - 5.57 Bq/L respectively. On the other hand, the concentrations of uranium-238 and thorium-232 were determined by using Energy Dispersive X-ray Fluorescence Spectrometry (EDXRF). The thorium concentrations are between 0.17 ppm to 0.28 ppm and uranium concentrations were 0.25 ppm to 0.31 ppm. The results show activity concentrations of radionuclides are slightly high near the river estuary. The Radium Equivalent, Absorbed Dose Rate, External Hazard Index, and Annual Effective Dose of {sup 226}Ra, {sup 228}Ra and {sup 40}K are also studied.« less
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
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.
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
Uranium disequilibrium in groundwater: An isotope dilution approach in hydrologic investigations
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.
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.
Time differences in the formation of meteorites as determined from the ratio of lead-207 to lead-206
Tatsumoto, M.; Knight, R.J.; Allegre, C.J.
1973-01-01
Measurements of the lead isotopic composition and the uranium, thorium, and lead concentrations in meteorites were made in order to obtain more precise radiometric ages of these members of the solar system. The newly determined value of the lead isotopic composition of Canyon Diablo troilite is as follows: 206Pb/204Pb = 9.307, 207Pb/204Pb = 10.294, and 208Pb/204Pb = 29.476. The leads of Angra dos Reis, Sioux County, and Nuevo Laredo achondrites are very radiogenic, the 206Pb/204Pb values are about 200, and the uranium-thorium-lead systems are nearly concordant. The ages of the meteorites as calculated from a single-stage 207Pb/206Pb isochron based on the newly determined primordial lead value and the newly reported 235U and 238U decay constants, are 4.528 ?? 10 9 years for Sioux County and Nuevo Laredo and 4.555 ?? 10 9 years for Angra dos Reis. When calculated with the uranium decay constants used by Patterson, these ages are 4.593 ?? 109 years and 4.620 ?? 109 years, respectively, and are therefore 40 to 70 ?? 106 years older than the 4.55 ?? 109 years age Patterson reported. The age difference of 27 ?? 106 years between Angra dos Reis and the other two meteorites is compatible with the difference between the initial 87Sr/86Sr ratio of Angra dos Reis and that of seven basaltic achondrites observed by Papanastassiou and Wasserburg. The time difference is also comparable to that determined by 129I-129Xe chronology. The ages of ordinary chondrites (H5 and L6) range from 4.52 to 4.57 ?? 109 years, and, here too, time differences in the formation of the parent bodies or later metamorphic events are indicated. Carbonaceous chondrites (C2 and C3) appear to contain younger lead components.
Bioaccessibility of U, Th and Pb in particulate matter from an abandoned uranium mine
NASA Astrophysics Data System (ADS)
Millward, Geoffrey; Foulkes, Michael; Henderson, Sam; Blake, William
2016-04-01
Currently, there are approximately 150 uranium mines in Europe at various stages of either operation, development, decommissioning, restoration or abandonment (wise-uranium.com). The particulate matter comprising the mounds of waste rock and mill tailings poses a risk to human health through the inadvertent ingestion of particles contaminated with uranium and thorium, and their decay products, which exposes recipients to the dual toxicity of heavy elements and their radioactive emissions. We investigated the bioaccessibility of 238U, 232Th and 206,214,210Pb in particulate samples taken from a contaminated, abandoned uranium mine in South West England. Sampling included a mine shaft, dressing floor and waste heap, as well as soils from a field used for grazing. The contaminants were extracted using the in-vitro Unified Bioaccessibility Research Group of Europe Method (UBM) in order to mimic the digestion processes in the human stomach (STOM) and the combined stomach and gastrointestinal tract (STOM+INT). Analyses of concentrations of U, Th and Pb in the extracts were by ICP-MS and the activity concentrations of radionuclides were determined on the same particles, before and after extraction, using gamma spectroscopy. 'Total' concentrations of U, Th and Pb for all samples were in the range 57 to 16,200, 0.28 to 3.8 and 69 to 4750 mg kg-1, respectively. For U and Pb the concentrations in the STOM fraction were lower than the total and STOM+INT fractions were even lower. However, for Th the STOM+INT fractions were higher than the STOM due to the presence of Th carbonate species within the gastrointestinal fluid. Activity concentrations for 214Pb and 210Pb, including total, STOM and STOM+INT, were in the range 180 to <1 Bq g-1 for the dressing floor and waste heap and 18 to <1 Bq g-1 for the grazing land. Estimates of the bioaccessible fractions (BAFs) of 238U in the most contaminated samples were 39% and 8% in the STOM and STOM+INT, respectively, whereas the respective BAFs for 232Th were 3% and 9%. For stable 206Pb the STOM and STOM+INT BAFs were 16% and 3% for the most contaminated samples, whereas those from the field had 44% in the STOM fraction and 17% in the STOM+INT fraction. The BAFs for 214Pb and 210Pb were the same as 206Pb. Dose estimates were made for the contaminants together with radioactive doses in order to assess potential risk to human health.
Hung, Nguyen Quoc; Chuong, Huynh Dinh; Vuong, Le Quang; Thanh, Tran Thien; Tao, Chau Van
2016-11-01
In this study, in situ gamma spectra using NaI(Tl) detector have been compared with the laboratory measurements by using HPGe detector on geological samples. The results for measuring naturally occurring terrestrial gamma radiation of 4 0 K and the decay series of 232 Th and, 238 U respectively of both detectors show a maximum deviation about 5%. The mass activities series from both detectors were checked for coherence using proficiency test procedure from the International Atomic Energy Agency. The reliability and precision pass for final scores for all the analytical determinations of are received "acceptable" for all radionuclides. Copyright © 2016 Elsevier Ltd. All rights reserved.
Wang, Xiao-Ping; Zhang, Ji-Long
2007-07-01
Twelve camphor (cinnamomum camphora) tree bark samples were collected from Hiroshima and Kyoto, and the matrix element composition and morphology of the outer surface of these camphor tree bark samples were studied by EDXS and SEM respectively. After a dry decomposition, DOWEX 1-X8 anion exchange resin was used to separate uranium from matrix elements in these camphor tree bark samples. Finally, 235U/238 U isotope ratios in purified uranium solutions were determined by MC-ICP-MS. It was demonstrated that the outer surface of these camphor tree bark samples is porous and rough, with Al, Ca, Fe, K, Mg, Si, C, O and S as its matrix element composition. Uranium in these camphor tree bark samples can be efficiently separated and quantitatively recovered from the matrix element composition. Compared with those collected from Kyoto, the camphor tree bark samples collected from Hiroshima have significantly higher uranium contents, which may be due to the increased aerosol mass concentration during the city reconstruction. Moreover, the 235 U/23.U isotope ratios in a few camphor tree bark samples collected from Hiroshima are slightly higher than 0.007 25.
Uranium-series coral ages from the US Atlantic Coastal Plain-the "80 ka problem" revisited
Wehmiller, J. F.; Simmons, K.R.; Cheng, H.; Edwards, R. Lawrence; Martin-McNaughton, J.; York, L.L.; Krantz, D.E.; Shen, C.-C.
2004-01-01
Uranium series coral ages for emergent units from the passive continental margin US Atlantic Coastal Plain (ACP) suggest sea level above present levels at the end of marine oxygen isotope stage (MIS) 5, contradicting age-elevation relations based on marine isotopic or coral reef models of ice equivalent sea level. We have reexamined this problem by obtaining high precision 230Th/238U and 231Pa/235U thermal ionization mass spectrometric ages for recently collected and carefully cleaned ACP corals, many in situ. We recognize samples that show no evidence for diagenesis on the basis of uranium isotopic composition and age concordance. Combining new and earlier data, among those ages close to or within the age range of MIS 5, over 85% cluster between 65 and 85 ka BP. Of the corals that we have analyzed, those that show the least evidence for diagenesis on the basis of uranium isotopic composition and age concordance have ages between 80 and 85 ka BP, consistent with a MIS 5a correlation. The units from which these samples have been collected are all emergent and have elevations within ???3-5m of those few units where early stage 5 (???125,000 ka BP) coral ages have been obtained. The ACP appears to record an unusual history of relative sea level throughout MIS 5, a history that is also apparent in the dated coral record for Bermuda. We speculate that this history is related to the regional (near-to intermediate-field) effects of ancestral Laurentide Ice sheets on last interglacial shorelines of the western North Atlantic. ?? 2004 Elsevier Ltd and INQUA. All rights reserved.
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.
An aerosol particle containing enriched uranium encountered in the remote upper troposphere.
Murphy, D M; Froyd, K D; Apel, E; Blake, D; Blake, N; Evangeliou, N; Hornbrook, R S; Peischl, J; Ray, E; Ryerson, T B; Thompson, C; Stohl, A
2018-04-01
We describe a submicron aerosol particle sampled at an altitude of 7 km near the Aleutian Islands that contained a small percentage of enriched uranium oxide. 235 U was 3.1 ± 0.5% of 238 U. During twenty years of aircraft sampling of millions of particles in the global atmosphere, we have rarely encountered a particle with a similarly high content of 238 U and never a particle with enriched 235 U. The bulk of the particle consisted of material consistent with combustion of heavy fuel oil. Analysis of wind trajectories and particle dispersion model results show that the particle could have originated from a variety of areas across Asia. The source of such a particle is unclear, and the particle is described here in case it indicates a novel source where enriched uranium was dispersed. Published by Elsevier Ltd.
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.
Active-Interrogation Measurements of Fast Neutrons from Induced Fission in Low-Enriched Uranium
DOE Office of Scientific and Technical Information (OSTI.GOV)
J. L. Dolan; M. J. Marcath; M. Flaska
2014-02-01
A detection system was designed with MCNPX-PoliMi to measure induced-fission neutrons from U-235 and U-238 using active interrogation. Measurements were then performed with this system at the Joint Research Centre (JRC) in Ispra, Italy on low-enriched uranium samples. Liquid scintillators measured induced fission neutron to characterize the samples in terms of their uranium mass and enrichment. Results are presented to investigate and support the use of organic liquid scintillators with active interrogation techniques to characterize uranium containing materials.
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.
Effect of low-dose ionizing radiation on luminous marine bacteria: radiation hormesis and toxicity.
Kudryasheva, N S; Rozhko, T V
2015-04-01
The paper summarizes studies of effects of alpha- and beta-emitting radionuclides (americium-241, uranium-235+238, and tritium) on marine microorganisms under conditions of chronic low-dose irradiation in aqueous media. Luminous marine bacteria were chosen as an example of these microorganisms; bioluminescent intensity was used as a tested physiological parameter. Non-linear dose-effect dependence was demonstrated. Three successive stages in the bioluminescent response to americium-241 and tritium were found: 1--absence of effects (stress recognition), 2--activation (adaptive response), and 3--inhibition (suppression of physiological function, i.e. radiation toxicity). The effects were attributed to radiation hormesis phenomenon. Biological role of reactive oxygen species, secondary products of the radioactive decay, is discussed. The study suggests an approach to evaluation of non-toxic and toxic stages under conditions of chronic radioactive exposure. Copyright © 2015 Elsevier Ltd. All rights reserved.
Mayer, Michael F.; Nattress, J.; Jovanovic, I.
2016-06-27
Detection of unique signatures of special nuclear materials is critical for their interdiction in a variety of nuclear security and nonproliferation scenarios. We report on the observation of delayed neutrons from fission of uranium induced in dual-particle active interrogation based on the 11B(d,n γ) 12C nuclear reaction. Majority of the fissions are attributed to fast fission induced by the incident quasi-monoenergetic neutrons. A Li-doped glass–polymer composite scintillation neutron detector, which displays excellent neutron/γ discrimination at low energies, was used in the measurements, along with a recoil-based liquid scintillation detector. Time- dependent buildup and decay of delayed neutron emission from 238Umore » were measured between the interrogating beam pulses and after the interrogating beam was turned off, respectively. Characteristic buildup and decay time profiles were compared to the common parametrization into six delayed neutron groups, finding a good agreement between the measurement and nuclear data. Furthermore, this method is promising for detecting fissile and fissionable materials in cargo scanning applications and can be readily integrated with transmission radiography using low-energy nuclear reaction sources.« less
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.
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}.
PIXE analysis of sand and soil from Ulaanbaatar and Karakurum, Mongolia
NASA Astrophysics Data System (ADS)
Markwitz, A.; Barry, B.; Shagjjamba, D.
2008-09-01
Twenty-one sand and soil samples were collected at the surface from 22 to 25 June 2007 at sampling sites from Ulaanbaatar to Karakurum, Mongolia. The sand samples were collected from constantly changing sand dunes which may still contain salt from prehistoric oceans. The dry sand and soil samples were processed for PIXE and PIGE analyses. A clear division between soils and sand become apparent in the silicon results. Concentrations of all bulk elements in human habitation samples and of Si, Al, K and Fe in dry lake/flood plain samples are similar to those in the soils and sands. Among elements which could be regarded as being at trace concentrations the average S concentration in the soils is 0.9 g kg-1 whereas it is not detected in the sand samples. Zinc and Cu concentrations are both higher in the soils than the sands and are strongly correlated. A surprising presence of uranium at a concentration of 350 mg kg-1 was detected in the PIXE measurement on one of the dry lake samples. Gamma spectrometry confirmed the presence of U in this sample and also at a lower level in a sample from the lake shore, but in none of the other samples. Further, the gamma spectrometry showed that 238U decay products were present only at a level corresponding to about 3 mg kg-1 U for a system in radioactive equilibrium, a figure which is typical for U in the earth's crust. Disequilibria between 238U and its decay products occur naturally but such a high degree of separation at high concentration would be unique if confirmed. PIXE and PIGE measurements of these samples highlight the difficulty in correlating trace element measurements with occurrence of indicators of sea salt in air particulate samples.
The estuarine chemistry and isotope systematics of 234,238U in the Amazon and Fly Rivers
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.
Biogeochemical aspects of uranium mineralization, mining, milling, and remediation
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.
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.
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.
Radiological Impact of Phosphogypsum Application in Agriculture
DOE Office of Scientific and Technical Information (OSTI.GOV)
Dias, Nivea M. P.; Caires, Eduardo F.; Pires, Luiz F.
2010-08-04
Phosphogypsum (PG) contains radionuclides from {sup 238}U and {sup 232}Th decay series. Due to the presence of these radionuclides, many countries restricted the use of PG in agriculture, however there is not such restriction in Brazil. The main objective of this work was to evaluate the impact of PG application on {sup 226}Ra ({sup 238}U) and {sup 228}Ra ({sup 232}Th) concentrations in soil. Gamma-spectrometry was carried out using HPGe detector. No increment of {sup 226}Ra and {sup 228}Ra was observed for increasing PG doses. Average values found for {sup 226}Ra and {sup 228}Ra were respectively 37 Bq kg{sup -1} andmore » 57 Bq kg{sup -1}. The results showed that the increasing PG doses in the specific conditions of the experiment did not cause a significant increment of radionuclides.« less
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.
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.
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.
NASA Technical Reports Server (NTRS)
Black, S.; Macdonald, R.; Kelly, M.
1993-01-01
U-series disequilibrium analyses have been conducted on samples from Olkaria rhyolite centers with ages being available for all but one center using both internal and whole rock isochrons. 67 percent of the rhyolites analyzed show U-Th disequilibrium, ranging from 27 percent excess thorium to 36 percent excess uranium. Internal and whole rock isochrons give crystallization/formation ages between 65 ka and 9 ka, in every case these are substantially older than the eruptive dates. The residence times of the rhyolites (U-Th age minus the eruption date) have decreased almost linearly with time, from 45 ka to 7 Ka suggesting a possible increase of activity within the system related to increased basaltic input. The long residence times are mirrored by large Rn-222 fluxes from the centers which cannot be explained by larger U contents.
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
β-γ and isomeric decay spectroscopy of 168Dy
NASA Astrophysics Data System (ADS)
Zhang, G. X.; Watanabe, H.; Kondev, F. G.; Lane, G. J.; Regan, P. H.; Söderström, P.-A.; Walker, P. M.; Kanaoka, H.; Korkulu, Z.; Lee, P. S.; Liu, J. J.; Nishimura, S.; Wu, J.; Yagi, A.; Ahn, D. S.; Alharbi, T.; Baba, H.; Browne, F.; Bruce, A. M.; Carroll, R. J.; Chae, K. Y.; Dombradi, Zs.; Doornenbal, P.; Estrade, A.; Fukuda, N.; Griffin, C.; Ideguchi, E.; Inabe, N.; Isobe, T.; Kanaya, S.; Kojouharov, I.; Kubo, T.; Kubono, S.; Kurz, N.; Kuti, I.; Lalkovski, S.; Lee, C. S.; Lee, E. J.; Lorusso, G.; Lotay, G.; Moon, C.-B.; Nishizuka, I.; Nita, C. R.; Odahara, A.; Patel, Z.; Phong, V. H.; Podolyák, Zs.; Roberts, O. J.; Sakurai, H.; Schaffner, H.; Shand, C. M.; Shimizu, Y.; Sumikama, T.; Suzuki, H.; Takeda, H.; Terashima, S.; Vajta, Zs.; Valiente-Dóbon, J. J.; Xu, Z. Y.
2018-05-01
This contribution will report on the experimental work on the level structure of 168Dy. The experimental data have been taken as part of the EURICA decay spectroscopy campaign at RIBF, RIKEN in November 2014. In the experiment, a 238U primary beam is accelerated up to 345 MeV/u with an average intensity of 12 pnA. The nuclei of interest are produced by in-flight fission of 238U impinging on Be target with a thickness of 5 mm. The excited states of 168Dy have been populated through the decay from a newly identified isomeric state and via the β decay from 168Tb. In this contribution, scientific motivations, experimental procedure and some preliminary results for this study are presented.
Background and Source Term Identification in Active Neutron Interrogation Methods
2011-03-24
interactions occurred to observe gamma ray peaks and not unduly increase simulation time. Not knowing the uranium enrichment modeled by Gozani, pure U...neutron interactions can occur. The uranium targets, though, should have increased neutron fluencies as the energy levels become below 2 MeV. This is...Assessment Monitor Site (TEAMS) at Kirtland AFB, NM. Iron (Fe-56), lead (Pb-207), polyethylene (C2H4 –– > C-12 & H-1), and uranium (U-235 and U-238) were
Microbial biogeochemistry of uranium mill tailings
Landa, Edward R.
2005-01-01
Uranium mill tailings (UMT) are the crushed ore residues from the extraction of uranium (U) from ores. Among the radioactive wastes associated with the nuclear fuel cycle, UMT are unique in terms of their volume and their limited isolation from the surficial environment. For this latter reason, their management and long-term fate has many interfaces with environmental microbial communities and processes. The interactions of microorganisms with UMT have been shown to be diverse and with significant consequences for radionuclide mobility and bioremediation. These radionuclides are associated with the U-decay series. The addition of organic carbon and phosphate is required to initiate the reduction of the U present in the groundwater down gradient of the mills. Investigations on sediment and water from the U-contaminated aquifer, indicates that the addition of a carbon source stimulates the rate of U removal by microbial reduction. Moreover, most attention with respect to passive or engineered removal of U from groundwaters focuses on iron-reducing and sulfate-reducing bacteria.
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.
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
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 radioactivity of the tar-sand deposits of Ondo State, Southwestern Nigeria
NASA Astrophysics Data System (ADS)
Fasasi, M. K.; Oyawale, A. A.; Mokobia, C. E.; Tchokossa, P.; Ajayi, T. R.; Balogun, F. A.
2003-06-01
A combination of gamma spectrometry and energy dispersive X-ray fluorescence was used to determine the presence and level of radioactivity of radionuclides in bituminous sand and overburden obtained from bituminous sand deposits in Ondo State Nigeria for the purpose of providing baseline data and assessing its impact on the environment. The radionuclides identified with reliable regularity belong to the decay series of naturally occurring radionuclides headed by 238U and 232Th. The non-decay series of naturally occurring 40K was found to be below the limit of detection. The average specific activity concentration values obtained for 214 Bi, 208Tl, and 226Ra in the overburden are 165.64±2.91, 150.25±2.91 and 60.97±2.27 Bq kg -1, respectively. The measured activity in the bituminous sand layer is so low that it can be said to be non-radioactive. The result of the EDXRF supports the presence of radioelements in the overburden, which are likely to be embedded in accessory minerals like zircon and tourmaline. Thus, surface exploration technique using soil-gas radon measurement will not yield the desired result. Furthermore, the level of radioelements and associated decay daughter 222Rn is not expected to cause any health hazard.
NASA Astrophysics Data System (ADS)
Guillong, M.; Schmitt, A. K.; Bachmann, O.
2015-04-01
Laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) of eight zircon reference materials and synthetic zircon-hafnon end-members indicate that corrections for abundance sensitivity and molecular zirconium sesquioxide ions (Zr2O3+) are critical for reliable determination of 230Th abundances in zircon. Other polyatomic interferences in the mass range 223-233 amu are insignificant. When corrected for abundance sensitivity and interferences, activity ratios of (230Th)/(238U) for the zircon reference materials we used average 1.001 ± 0.010 (1σ error; mean square of weighted deviates MSWD = 1.45; n = 8). This includes the 91500 and Plešovice zircons, which were deemed unsuitable for calibration of (230Th)/(238U) by Ito (2014). Uranium series zircon ages generated by LA-ICP-MS without mitigating (e.g., by high mass resolution) or correcting for abundance sensitivity and molecular interferences on 230Th such as those presented by Ito (2014) are potentially unreliable.
Urey, Harold Clayton (1893-1981)
NASA Astrophysics Data System (ADS)
Murdin, P.
2000-11-01
Chemist, born in Walkerton, Indiana, Nobel prizewinner for Chemistry in 1934 `for his discovery of heavy hydrogen'. It was at Columbia University that he isolated the isotope deuterium by distilling liquid hydrogen; in the Second World War, he directed the effort to separate uranium-235 from uranium-238 for the atomic bomb. At the University of Chicago, he worked on the origin of the elements, th...
Stability Estimation of ABWR on the Basis of Noise Analysis
NASA Astrophysics Data System (ADS)
Furuya, Masahiro; Fukahori, Takanori; Mizokami, Shinya; Yokoya, Jun
In order to investigate the stability of a nuclear reactor core with an oxide mixture of uranium and plutonium (MOX) fuel installed, channel stability and regional stability tests were conducted with the SIRIUS-F facility. The SIRIUS-F facility was designed and constructed to provide a highly accurate simulation of thermal-hydraulic (channel) instabilities and coupled thermalhydraulics-neutronics instabilities of the Advanced Boiling Water Reactors (ABWRs). A real-time simulation was performed by modal point kinetics of reactor neutronics and fuel-rod thermal conduction on the basis of a measured void fraction in a reactor core section of the facility. A time series analysis was performed to calculate decay ratio and resonance frequency from a dominant pole of a transfer function by applying auto regressive (AR) methods to the time-series of the core inlet flow rate. Experiments were conducted with the SIRIUS-F facility, which simulates ABWR with MOX fuel installed. The variations in the decay ratio and resonance frequency among the five common AR methods are within 0.03 and 0.01 Hz, respectively. In this system, the appropriate decay ratio and resonance frequency can be estimated on the basis of the Yule-Walker method with the model order of 30.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sasaki, Takayuki, E-mail: sasaki@nucleng.kyoto-u.ac.jp; Rajib, Mohammad; Akiyoshi, Masafumi
2015-06-15
The present study reports the likely first attempt of separating radioactive minerals for estimation of activity concentration in the beach placer sands of Bangladesh. Several sand samples from heavy mineral deposits located at the south-eastern coastal belt of Bangladesh were processed to physically upgrade their radioactivity concentrations using plant and laboratory equipment. Following some modified flow procedure, individual fractions were separated and investigated using gamma-ray spectrometry and powder-XRD analysis. The radioactivity measurements indicated contributions of the thorium and uranium radioactive series and of {sup 40}K. The maximum values of {sup 232}Th and {sup 238}U, estimated from the radioactivity of {supmore » 208}Tl and {sup 234}Th in secular equilibrium, were found to be 152,000 and 63,300 Bq/kg, respectively. The fraction of the moderately conductive part in electric separation contained thorium predominantly, while that of the non-conductive part was found to be uranium rich. The present arrangement of the pilot plant cascade and the fine tuning of setting parameters were found to be effective and economic separation process of the radioactive minerals from placer sands in Bangladesh. Probable radiological impacts and extraction potentiality of such radioactive materials are also discussed.« less
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.
Graphic and algebraic solutions of the discordant lead-uranium age problem
Stieff, L.R.; Stern, T.W.
1961-01-01
Uranium-bearing minerals that give lead-uranium and lead-lead ages that are essentially in agreement, i.e. concordant, generally are considered to have had a relatively simple geologic history and to have been unaltered since their deposition. The concordant ages obtained on such materials are, therefore, assumed to approach closely the actual age of the minerals. Many uranium-bearing samples, particularly uranium ores, give the following discordant age sequences; Pb206 U238 < Pb207 U235 ??? Pb207 Pb206 or, less frequently, Pb207 Pb206 ??? Pb207 U235 < Pb206 U238. These discordant age sequences have been attributed most often to uncertainties in the common lead correction, selective loss of radio-active daughter products, loss or gain of lead or uranium, or contamination by an older generation of radiogenic lead. The evaluation of discordant lead isotope age data may be separated into two operations. The first operation, with which this paper is concerned, is mechanical in nature and involves the calculation of the different possible concordant ages corresponding to the various processes assumed to have produced the discordant ages. The second operation is more difficult to define and requires, in part, some personal judgement. It includes a synthesis of the possible concordant age solutions with other independent geologic and isotopic evidence. The concordant age ultimately chosen as most acceptable should be consistent not only with the known events in the geologic history of the area, the age relations of the enclosing rocks, and the mineralogic and paragenetic evidence, but also with other independent age measurements and the isotopic data obtained on the lead in related or associated non-radioactive minerals. The calculation of the possible concordant ages from discordant age data has been greatly simplified by Wetherill's graphical method of plotting the mole ratios of radiogenic Pb206 U238 ( N206 N238) vs. radiogenic Pb207 U235 ( N207 N235) after correcting for the contaminating common Pb206 and Pb207. The linear relationships noted in this graphical procedure have been extended to plots of the mole ratios of total Pb206 U238 ( tN206 N238) vs. total Pb207 U235 ( tN207 N235). This modification permits the calculation of concordant ages for unaltered samples using only the Pb207 Pb206 ratio of the contaminating common lead. If isotopic data are available for two samples of the same age, x and y, from the same or related deposits or outcrops, graphs of the normalized difference ratios [ ( N206 N204)x - ( N206 N204)y ( N238 N204)x -( N238 N204)y] vs. [ ( N207 N204)x - ( N207 N204)y ( N235 N204)x -( N235 N204)y] can give concordant ages corrected for unknown amounts of a common lead with an unknown Pb207/ Pb206 ratio. (If thorium is absent the difference ratios may be normalized with the more abundant index isotope, Pb208.) Similar plots of tho normalized, difference ratios for three genetically related samples (x - y) and(x - z), will give concordant ages corrected, in addition, for either one unknown period of past alteration or initial contamination by an older generation of radiogenic lead of unknown Pb207/Pb206 ratio. Practical numerical solutions for many of tho concordant age calculations are not currently available. However, the algebraic equivalents of these new graphical methods give equations which may be programmed for computing machines. For geologically probable parameters the equations of higher order have two positive real roots that rapidly converge on the exact concordant ages corrected for original radiogenic lead and for loss or gain of lead or uranium. Modifications of these general age equations expanded only to the second degree have been derived for use with desk calculators. These graphical and algebraic methods clearly suggest both the type and minimum number of samples necessary for adequate mathematical analysis of discordant lead isotope age data. This mathematical treatment also makes it clear t
Consequences of slow growth for 230Th/U dating of Quaternary opals, Yucca Mountain, NV, USA
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.
Szabo, Zoltan; Zapecza, Otto S.; Oden, Jeannette H.; Rice, Donald E.
2005-01-01
A field sampling experiment was designed using low-flow purging with a portable pump and sample-collection equipment for the collection of water and sediment samples from observation wells screened in the Kirkwood-Cohansey aquifer system to determine radionuclide or trace-element concentrations for various size fractions. Selected chemical and physical characteristics were determined for water samples from observation wells that had not been purged for years. The sampling was designed to define any particulate, colloidal, and solution-phase associations of radionuclides or trace elements in ground water by means of filtration and ultrafiltration techniques. Turbidity was monitored and allowed to stabilize before samples were collected by means of the low-flow purging technique rather than by the traditional method of purging a fixed volume of water at high-flow rates from the observation well. A minimum of four water samples was collected from each observation well. The samples of water from each well were collected in the following sequence. (1) A raw unfiltered sample was collected within the first minutes of pumping. (2) A raw unfiltered sample was collected after at least three casing volumes of water were removed and turbidity stabilized. (3) A sample was collected after the water was filtered with a 0.45-micron filter. (4) A sample was collected after the water passed through a 0.45-micron filter and a 0.003-micron tangential-flow ultrafilter in sequence. In some cases, a fifth sample was collected after the water passed through a 0.45-micron filter and a 0.05-micron filter in sequence to test for colloids of 0.003 microns to 0.05 microns in size. The samples were analyzed for the concentration of manmade radionuclides plutonium-238 and -239 plus -240, and americium-241. The samples also were analyzed for concentrations of uranium-234, -235, and -238 to determine whether uranium-234 isotope enrichment (resulting from industrial processing) is present. A subset of samples was analyzed for concentrations of thorium-232, -230, and -228 to determine if thorium-228 isotope enrichment, also likely to result from industrial processing, is present. Concentrations of plutonium isotopes and americium-241 in the water samples were less than 0.1 picocurie per liter, the laboratory reporting level for these manmade radionuclides, with the exception of one americium-241 concentration from a filtered sample. A sequential split sample from the same well did not contain a detectable concentration of americium-241, however. Other filtered and unfiltered samples of water from the same well did not contain quantities of americium-241 nearly as high as 0.1 pCi/L. Therefore, the presence of americium-241 in a quantifiable concentration in water samples from this well could not be confirmed. Neither plutonium nor americium was detected in samples of settled sediment collected from the bottom of the wells. Concentrations of uranium isotopes (maximum of 0.05 and 0.08 picocuries per liter of uranium-238 and uranium-234, respectively) were measurable in unfiltered samples of turbid water from one well and in the settled bottom sediment from 6 wells (maximum concentrations of 0.25 and 0.20 picocuries per gram of uranium-238 and uranium-234, respectively). The uranium-234/uranium-238 isotopic ratio was near 1:1, which indicates natural uranium. The analytical results, therefore, indicate that no manmade radionuclide contamination is present in any of the well-bottom sediments, or unfiltered or filtered water samples from any of the sampled wells. No evidence of manmade radionuclide contamination was observed in the aquifer as settled or suspended particulates, colloids, or in the dissolved phase.
Abundances of uranium, thorium, and potassium for some Australian crystalline rocks
Bunker, Carl Maurice; Bush, C.A.; Munroe, Robert J.; Sass, J.H.
1975-01-01
This report contains a tabulation of the basic radioelement and radiogenic heat data obtained during an Australian National University (ANU) - United States Geological Survey (USGS) heat-flow project, directed jointly by J. C. Jaeger (ANU) and J. H. Sass (USGS). Most samples were collected during the periods June through September, 1971 and 1972. The measurements were made subsequently by two of us (C. M. Bunker and C. A. Bush) using the gamma-ray spec trometric techniques described by Bunker and Bush (1966, 1967). Interpreting the spectra for quantitative analyses of the radioelements was accomplished with an iterative leastsquares computer program modified from one by Schonfeld (1966). Uranium content determined by gamma-ray spectrometry is based on a measurement of the daughter products of 226Ra. Equilibrium in the uranium-decay series was assumed for these analyses . Throughout the report, when U content is stated, radium-equivalent uranium is implied. The coefficient of variation for the accuracy of the radioelement data, when compared to ana lyses by isotope dilution and flame photometry is about 3 percent for radium-equivalent uranium and thorium and about 1 percent for potassium. These percentages are in addition to minimum standard deviations of about 0.05 ppm for U and Th, and about 0.03 percent for K.
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
Estimation of uranium migration parameters in sandstone aquifers.
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.
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.
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.
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
NASA Astrophysics Data System (ADS)
Ghosal, S.; Agrahari, S.; Guin, R.; Sengupta, D.
2017-01-01
A radioelemental assemblage assessment of two beaches of Odisha is performed for the first time. The radiation is measured in two ways, both on field with the help of a hand held environmental survey meter and in the laboratory, where the concentrations of radionuclide's 238U, 232Th and 4K have been determined with the help of High Purity Germanium detector (HPGe). Mineralogical analysis of selected samples has been performed with the help of X-Ray Fluorescence Spectrometry (XRF). A marked difference between the concentration of Uranium (274 Bq kg-1) and Thorium (2489 Bq kg-1) is observed and discussed based on the geology of the area. The placer deposits showing an enrichment of thorium can be an important source of nuclear fuel for the thorium based nuclear reactors. The ratio of thorium and uranium concentrations gives us an idea about the coastal processes associated with the beach. Statistical analysis of the data shows a positive correlation between 238U and 232Th and a strong negative correlation is indicated between 4 K and 238U, 232Th. A cross plot between the equivalent thorium and the equivalent uranium and the equivalent thorium and potassium, represents the nature of deposition and its association with the heavy mineral along with the radioactive elements. Heavy minerals exhibit an increasing trend towards Northeast-Southwest along the south eastern coast of India.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Scott, B.R.; Muggenburg, B.A.; Welsh, C.A.
The alpha emitter plutonium-238 ({sup 238}Pu), which is produced in uranium-fueled, light-water reactors, is used as a thermoelectric power source for space applications. Inhalation of a mixed oxide form of Pu is the most likely mode of exposure of workers and the general public. Occupational exposures to {sup 238}PuO{sub 2} have occurred in association with the fabrication of radioisotope thermoelectric generators. Organs and tissue at risk for deterministic and stochastic effects of {sup 238}Pu-alpha irradiation include the lung, liver, skeleton, and lymphatic tissue. Little has been reported about the effects of inhaled {sup 238}PuO{sub 2} on peripheral blood cell countsmore » in humans. The purpose of this study was to investigate hematological responses after a single inhalation exposure of Beagle dogs to alpha-emitting {sup 238}PuO{sub 2} particles and to extrapolate results to humans.« less
Two-dimensional fluorescence spectroscopy of uranium isotopes in femtosecond laser ablation plumes
DOE Office of Scientific and Technical Information (OSTI.GOV)
Phillips, Mark C.; Brumfield, Brian E.; LaHaye, Nicole
Here, we demonstrate measurement of uranium isotopes in femtosecond laser ablation plumes using two-dimensional fluorescence spectroscopy (2DFS). The high-resolution, tunable CW-laser spectroscopy technique clearly distinguishes atomic absorption from 235U and 238U in natural and highly enriched uranium metal samples. We present analysis of spectral resolution and analytical performance of 2DFS as a function of ambient pressure. Simultaneous measurement using time-resolved absorption spectroscopy provides information on temporal dynamics of the laser ablation plume and saturation behavior of fluorescence signals. The rapid, non-contact measurement is promising for in-field, standoff measurements of uranium enrichment for nuclear safety and security.
Two-dimensional fluorescence spectroscopy of uranium isotopes in femtosecond laser ablation plumes
DOE Office of Scientific and Technical Information (OSTI.GOV)
Phillips, Mark C.; Brumfield, Brian E.; LaHaye, Nicole L.
We demonstrate measurement of uranium isotopes in femtosecond laser ablation plumes using two-dimensional fluorescence spectroscopy (2DFS). The high-resolution, tunable CW-laser spectroscopy technique clearly distinguishes atomic absorption from 235U and 238U in natural and highly enriched uranium metal samples. We present analysis of spectral resolution and analytical performance of 2DFS as a function of ambient pressure. Simultaneous measurement using time-resolved absorption spectroscopy provides information on temporal dynamics of the laser ablation plume and saturation behavior of fluorescence signals. The rapid, non-contact measurement is promising for in-field, standoff measurements of uranium enrichment for nuclear safety and security applications.
Two-dimensional fluorescence spectroscopy of uranium isotopes in femtosecond laser ablation plumes
Phillips, Mark C.; Brumfield, Brian E.; LaHaye, Nicole; ...
2017-06-19
Here, we demonstrate measurement of uranium isotopes in femtosecond laser ablation plumes using two-dimensional fluorescence spectroscopy (2DFS). The high-resolution, tunable CW-laser spectroscopy technique clearly distinguishes atomic absorption from 235U and 238U in natural and highly enriched uranium metal samples. We present analysis of spectral resolution and analytical performance of 2DFS as a function of ambient pressure. Simultaneous measurement using time-resolved absorption spectroscopy provides information on temporal dynamics of the laser ablation plume and saturation behavior of fluorescence signals. The rapid, non-contact measurement is promising for in-field, standoff measurements of uranium enrichment for nuclear safety and security.
Simulated fissioning of uranium and testing of the fission-track dating method
McGee, V.E.; Johnson, N.M.; Naeser, C.W.
1985-01-01
A computer program (FTD-SIM) faithfully simulates the fissioning of 238U with time and 235U with neutron dose. The simulation is based on first principles of physics where the fissioning of 238U with the flux of time is described by Ns = ??f 238Ut and the fissioning of 235U with the fluence of neutrons is described by Ni = ??235U??. The Poisson law is used to set the stochastic variation of fissioning within the uranium population. The life history of a given crystal can thus be traced under an infinite variety of age and irradiation conditions. A single dating attempt or up to 500 dating attempts on a given crystal population can be simulated by specifying the age of the crystal population, the size and variation in the areas to be counted, the amount and distribution of uranium, the neutron dose to be used and its variation, and the desired ratio of 238U to 235U. A variety of probability distributions can be applied to uranium and counting-area. The Price and Walker age equation is used to estimate age. The output of FTD-SIM includes the tabulated results of each individual dating attempt (sample) on demand and/or the summary statistics and histograms for multiple dating attempts (samples) including the sampling age. An analysis of the results from FTD-SIM shows that: (1) The external detector method is intrinsically more precise than the population method. (2) For the external detector method a correlation between spontaneous track count, Ns, and induced track count, Ni, results when the population of grains has a stochastic uranium content and/or when the counting areas between grains are stochastic. For the population method no correlation can exist. (3) In the external detector method the sampling distribution of age is independent of the number of grains counted. In the population method the sampling distribution of age is highly dependent on the number of grains counted. (4) Grains with zero-track counts, either in Ns or Ni, are in integral part of fissioning theory and under certain circumstances must be included in any estimate of age. (5) In estimating standard error of age the standard error of Ns and Ni and ?? must be accurately estimated and propagated through the age equation. Several statistical models are presently available to do so. ?? 1985.
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.
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.
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 isotopes and dissolved organic carbon in loess permafrost: Modeling the age of ancient ice
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.
NASA Astrophysics Data System (ADS)
2001-02-01
First Reading of a Basic Cosmic Chronometer with UVES and the VLT Summary Most astronomers would agree that the age of the Universe - the time elapsed since the "Big Bang" - is one of the " holy grails of cosmology ". Despite great efforts during recent years, the various estimates of this basic number have resulted in rather diverse values. When derived from current cosmological models, it depends on a number of theoretical assumptions that are not very well constrained by the incomplete available observational data. At present, a value in the range of 10-16 billion years [1] is considered most likely. But now, an international team of astronomers [2] has used the powerful ESO Very Large Telescope (VLT) and its very efficient spectrograph UVES to perform a unique measurement that paves the way for a new and more accurate determination of the age of the Universe. They measured for the first time the amount of the radioactive isotope Uranium-238 in a star that was born when the Milky Way, the galaxy in which we live, was still forming. It is the first measurement ever of uranium outside the Solar System . This method works in a way similar to the well-known Carbon-14 dating in archaeology, but over much longer times. Ever since the star was born, the Uranium "clock" has ticked away over the eons, unaffected by the turbulent history of the Milky Way. It now reads 12.5 billion years . Since the star obviously cannot be older than the Universe, it means that the Universe must be older than that . Although the stated uncertainty is still about 25% or about ±3 billion years, this is only to a minor extent due to the astronomical observation. The main problem is the current absence of accurate knowledge of some of the basic atomic and nuclear properties of the elements involved. However, further laboratory work will greatly improve this situation and a more accurate value for the age of the star and implicitly, for the Universe, should therefore be forthcoming before long . This important result is reported in the international research journal Nature in the issue of February 8, 2001. PR Photo 05a/01 : The 12.5-billion-year old star CS 31082-001. PR Photo 05b/01 : The telltale spectral line in CS 31082-001 - the first detection of uranium outside the Solar System . Heavy elements in stars While hydrogen, helium and lithium were produced during the Big Bang, all heavier elements result from nuclear reactions in the interiors of stars. When stars die, heavy-element enriched matter is dispersed into surrounding space and will later be incorporated in the next generations of stars. In fact, the gold in the ring on your finger was produced in an exploding star and deposited in the interstellar cloud from which the Sun and its planets were later formed. Thus, the older a star is, the lower is generally its content of heavy elements like iron and other metals. Measurements have shown that old stars that are members of large agglomerations known as globular clusters are normally quite "metal-poor"- their metal-content ranges down to about 1/200 of that of the Sun, in which these metals constitute only 2% of the total mass, the rest being still in the form of hydrogen and helium. Very old stars in the Milky Way galaxy After decades of mostly fruitless efforts, a large spectral survey by American astronomer Timothy C. Beers and his collaborators has recently uncovered hundreds of stars with much lower metal content than even the globular clusters, in some cases only 1/10,000 of the solar value. It is evident that these extremely metal-poor stars must have formed during the very infancy of the Milky Way, an important, but still poorly understood phase in the life of our galaxy. These particular stars exhibit a great variety of element abundances that may ultimately throw more light on the processes at work during this early period. As a step in this direction, an international team of astronomers [2] decided to study these stars in much more detail. They were awarded observing time for a Large Programme in 2000-2001 with the powerful combination of the ESO VLT and its very efficient high-dispersion spectrograph UVES. The first observations have been carried out and, not unexpectedly, have already proven to be a true gold mine of new information. Cosmochronology with radioactive isotopes It is possible to make a fundamental determination of the age of a star that is quite independent of stellar evolution models, provided it contains a suitable long-lived radioactive isotope [3]. The use of a "radioactive chronometer" depends on the measurement of the abundance of the radioactive isotope, as compared to a stable one. This technique is analogous to the Carbon-14 dating method that has been so successful in archaeology over time spans of up to a few tens of thousands of years. In astronomy, however, this technique must obviously be applied to vastly longer time scales. For the method to work well, the right choice of radioactive isotope is very critical. Contrary to stable elements that formed at the same time, the abundance of a radioactive (unstable) isotope decreases all the time. The faster the decay, the less there will be left of the radioactive isotope after a certain time, the greater will be the abundance difference when compared to a stable isotope, and the more accurate is the resulting age. Yet, for the clock to remain useful, the radioactive element must not decay too fast - there must still be enough left of it to allow an accurate measurement, even after several billion years. Thorium and Uranium clocks This leaves only two possible isotopes for astronomical measurements, thorium ( 232 Th or Thorium-232, with a half-life of 14.05 billion years [4]) and uranium ( 238 U or Uranium-238, half-life 4.47 billion years). Several age determinations have been made by means of the Thorium-232 isotope. Its strongest spectral line is measurable with current telescopes in a handful of comparatively bright stars, including the Sun. However, the decay is really too slow to provide sufficiently accurate time measurements. It takes around 47 billion years for this isotope to decay by a factor of 10, and with a typical measuring uncertainty of 25%, the resulting age uncertainty is about 4-5 billion years, or approx. one third of the age of the Universe. This slow-moving clock runs forever, but is hard to read accurately! The faster decay of Uranium-238 would make it a much more precise cosmic clock. However, because uranium is the rarest of all normal elements, its spectral lines in stars are always very weak; if visible at all, they normally drown entirely in a vast ocean of stronger spectral lines from more abundant elements. Nevertheless, this is exactly where the low abundance of heavier elements in very old stars comes to the rescue. In the stars that were studied by the present team at the VLT, with typically 1000 times less of the common elements than in the Sun, the predominance of the maze of atomic and molecular lines in the spectrum is greatly reduced. The lines of rare elements like uranium therefore stand a real chance of being measurable. This is particularly so, if for some reason uranium atoms were preferentially retained in the debris of those early supernova explosions that also created the iron-group elements we see in the stars today. The uranium line in CS 31082-001 ESO PR Photo 05a/01 ESO PR Photo 05a/01 [Preview - JPEG: 337 x 400 pix - 32k] [Normal - JPEG: 674 x 800 pix - 120k] Caption : PR Photo 05a/01 displays the Milky Way star field around CS 31082-001 , the 12th-magnitude star at the centre. The "cross" is caused by reflections in the telescope optics, a typical effect for relatively bright stars. Technical information about this photo is available below. ESO PR Photo 05b/01 ESO PR Photo 05b/01 [Preview - JPEG: 501 x 400 pix - 42k] [Normal - JPEG: 1001 x 800 pix - 128k] [Full-Res - JPEG: 1502 x 1200 pix - 200k] Caption : PR Photo 05b/01 The observed spectrum (dots) of the old star CS 31082-001 in the region of the uranium (U II) line at 385.96 nm. The origin of some of the other spectral lines in the region is also indicated (e.g. iron, neodymium). The synthetic spectrum (thin line) was computed for the adopted abundances of the stable elements and for four different values of the abundance (by number) of uranium atoms in the atmosphere of the star. The uppermost line (corresponding to no uranium at all) clearly does not fit the observed spectrum at all. The best fit is provided by the middle (red) line, representing a uranium abundance of approximately 6% of the solar value - see also the text. Technical information about this diagramme is available below. The excitement of the astronomers was great when they inspected the first spectrum of the 12th-magnitude programme star CS 31082-001 ! It showed what is probably the richest spectrum of rare, heavy elements ever seen. In particular, the faint lines of these elements were unusually free of interference from the lines of the iron-group elements which are indeed only 1/800 as abundant in this star as in the Sun, and by molecular lines (of CH and CN), often quite numerous even in such low-metallicity stars. While only one or at most two thorium lines have ever been measured in any other stars, no less than 14 thorium lines are seen in the spectrum of CS 31082-001 . Indeed, there is such a wealth of lines of other rare and precious metals that this spectrum is a real astronomers' treasure box. And best of all, the long sought-after line of singly ionized uranium is clearly detected at its rest wavelength of 389.59 nm in the near-ultraviolet region of the spectrum, cf. PR Photo 05b/01 ! Not surprisingly, the uranium line is still quite weak. After all, uranium is the rarest of elements to begin with and it has further decayed by a factor of eight since this star was born. Moreover, even in this low metal-abundance star, the near-UV spectrum remains rather rich in other lines. The accurate measurement of this faint spectral line therefore places extreme demands on the acuity (resolving power) and efficiency of the spectrograph and the light-gathering power of the telescope. The VLT and UVES have been built as the world-leading combination of these observational assets, and the spectra obtained of this comparatively faint star (magnitude 12, i.e. 500 times fainter than what can be seen with the unaided eye) are absolutely superb - indeed of a quality which until recently was reserved for naked-eye stars only. Despite its faintness, the uranium line can therefore be measured with very good accuracy. The age of CS 31082-001 A detailed analysis, using model atmospheres and synthetic spectrum calculations, shows that all the heaviest stable elements follow closely the abundance pattern seen in the Sun, but at a level of about 12% of the corresponding solar abundances [5]. The measurements also show that the thorium and uranium abundances are somewhat lower than this - of the order of 9% and 6% of the solar values, respectively. Since these two elements were formed by the same atomic processes as their stable neighbours in the periodic table, this means that radioactive decay has progressed further in CS 31082-001 than in the Sun. Different models of the element production in supernova explosions predict somewhat different production ratios between the stable and radioactive isotopes, leading to age estimates for this star in the range 11-16 billion years. The most likely age of CS 31082-001 is 12.5 billion years . The Universe is older than the star, hence it must be older than 12.5 billion years. Improved age determination soon possible Given the faster decay rate of Uranium-238, the measuring uncertainty for the stellar uranium line corresponds to an age uncertainty of only ±1.5 Gyr. This can be further reduced with even better spectra of CS 31082-001 and/or with the discovery and observation of other similar stars. However, for the immediate future, the accuracy of this age determination does not really depend on the VLT spectrum. For the time being, the real problems are the present uncertainties in the available laboratory data for uranium by means of which the measured line strengths are converted into element abundances. In addition, the nuclear-physics calculations of the initial isotope production ratios introduce errors that are larger than those of the spectral observation. Thus, improved measurements of those physical data are necessary in order to read more accurately the cosmic clock in CS 31082-001 from the existing observational data. The relevant laboratory measurements are now underway at the CEA, Saclay, France, and the University of Lund, Sweden. In the meantime, the team is trying to find other stars like CS 31082-001 . There may not be many, but if the uranium line can be seen and measured in more spectra, it will also become possible to judge whether those very old stars, as surmised, are all of about the same age, i.e. that of our Milky Way galaxy. More information The research described in this Press Release is reported in a research article ("Measurement of stellar age from uranium decay"), that appears in the international research journal Nature on Thursday, February 8, 2001. Notes [1]: 1 billion = 1,000 million. [2]: The team members are: Roger Cayrel (P.I.), Francois Spite and Monique Spite (all Observatoire de Paris, France), Vanessa Hill and Francesca Primas (ESO), Johannes Andersen and Birgitta Nordström (Copenhagen and Lund Observatories, Denmark and Sweden), Timothy C. Beers (Michigan State Univ., USA), Piercarlo Bonifacio and Paolo Molaro (Trieste, Italy), Bertrand Plez (Montpellier, France), and Beatriz Barbuy (Univ. of Sao Paulo, Brazil). [3]: Isotopes of a natural element contain different numbers of neutrons in the nuclei, in addition to a certain number of protons that characterize that particular element. Some isotopes are "radioactive", i.e. with time they are transformed into other elements or isotopes. Other isotopes are stable over exceedingly long periods of time. Uranium-238 contains 92 protons and 146 neutrons. [4]: The "half-life" of an isotope indicates the time after which half the atoms have decayed. After another time interval of this length has passed, only 25% of the original isotope is left, etc. [5]: As the iron abundance in CS 31082-001 is only 0.12% (1/800) of that in the Sun, this means that, relative to iron and similar, lighter elements, the heaviest elements in that star are approximately 100 times "overabundant". Their spectral lines, again in relative terms, are correspondingly stronger - this is of crucial importance for the present, difficult measurements. Technical information about the photos PR Photo 05a/01 is reproduced from the STScI Digitized Sky Survey (© 1993, 1994, AURA, Inc. - original plate material by Royal Observatory Edinburgh and the Anglo-Australian Observatory - All Rights Reserved) and based on blue-sensitive photographic data obtained using the UK Schmidt Telescope at Siding Spring (Australia). The comparatively empty sky field is located at high southern (-76°) galactic latitude and measures 7 x 7 arcmin 2 and. PR Photo 05b/01 is reproduced from a spectrum of CS 31082-001 , obtained in October 2000 with the UVES high-dispersion spectrograph at the VLT 8.2-m KUEYEN telescope at Paranal. The exposure lasted 4 hours, at a spectral resolution of approx. 75,000 and with a S/N-ratio of about 300. The lines are identified and three synthetic spectra, with different U-abundances, are drawn to illustrate the fit.
NASA Astrophysics Data System (ADS)
Du, Q.; Lin, S. T.; He, H. T.; Liu, S. K.; Tang, C. J.; Wang, L.; Wong, H. T.; Xing, H. Y.; Yue, Q.; Zhu, J. J.
2018-04-01
A measurement is reported for the response to charged particles of a liquid scintillator named EJ-335 doped with 0.5% gadolinium by weight. This liquid scintillator was used as the detection medium in a neutron detector. The measurement is based on the in-situ α-particles from the intrinsic Uranium and Thorium contamination in the scintillator. The β–α and the α–α cascade decays from the U/Th decay chains were used to select α-particles. The contamination levels of U/Th were consequently measured to be (5.54±0.15)× 10‑11 g/g, (1.45±0.01)× 10‑10 g/g and (1.07±0.01)× 10‑11 g/g for 232Th, 238U and 235U, respectively, assuming secular equilibrium. The stopping power of α-particles in the liquid scintillator was simulated by the TRIM software. Then the Birks constant, kB, of the scintillator for α-particles was determined to be (7.28±0.23) mg/(cm2ṡMeV) by Birks' formulation. The response for protons is also presented assuming the kB constant is the same as for α-particles.
PLANTS AS BIO-MONITORS FOR 137CS, 238PU, 239, 240PU AND 40K AT THE SAVANNAH RIVER SITE
DOE Office of Scientific and Technical Information (OSTI.GOV)
Caldwell, E.; Duff, M.; Ferguson, C.
2010-12-16
The nuclear fuel cycle generates a considerable amount of radioactive waste, which often includes nuclear fission products, such as strontium-90 ({sup 90}Sr) and cesium-137 ({sup 137}Cs), and actinides such as uranium (U) and plutonium (Pu). When released into the environment, large quantities of these radionuclides can present considerable problems to man and biota due to their radioactive nature and, in some cases as with the actinides, their chemical toxicity. Radionuclides are expected to decay at a known rate. Yet, research has shown the rate of elimination from an ecosystem to differ from the decay rate due to physical, chemical andmore » biological processes that remove the contaminant or reduce its biological availability. Knowledge regarding the rate by which a contaminant is eliminated from an ecosystem (ecological half-life) is important for evaluating the duration and potential severity of risk. To better understand a contaminants impact on an environment, consideration should be given to plants. As primary producers, they represent an important mode of contamination transfer from sediments and soils into the food chain. Contaminants that are chemically and/or physically sequestered in a media are less likely to be bio-available to plants and therefore an ecosystem.« less
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.
Prospects for improved understanding of isotopic reactor antineutrino fluxes
NASA Astrophysics Data System (ADS)
Gebre, Y.; Littlejohn, B. R.; Surukuchi, P. T.
2018-01-01
Predictions of antineutrino fluxes produced by fission isotopes in a nuclear reactor have recently received increased scrutiny due to observed differences in predicted and measured inverse beta decay (IBD) yields, referred to as the "reactor antineutrino flux anomaly." In this paper, global fits are applied to existing IBD yield measurements to produce constraints on antineutrino production by individual plutonium and uranium fission isotopes. We find that fits including measurements from highly
Vandenhove, H; Van Hees, M; Wannijn, J; Wouters, K; Wang, L
2007-01-01
The present study aimed to quantify the influence of soil parameters on uranium uptake by ryegrass. Ryegrass was established on eighteen distinct soils, spiked with (238)U. Uranium soil-to-plant transfer factors (TF) ranged from 0.0003 to 0.0340kgkg(-1). There was no significant relation between the U soil-to-plant transfer (or total U uptake or flux) and the uranium concentration in the soil solution or any other soil factor measured, nor with the U recovered following selective soil extractions. Multiple linear regression analysis resulted in a significant though complex model explaining up to 99% of variation in TF. The influence of uranium speciation on uranium uptake observed was featured: UO(2)(+2), uranyl carbonate complexes and UO(2)PO(4)(-) seem the U species being preferentially taken up by the roots and transferred to the shoots. Improved correlations were obtained when relating the uranium TF with the summed soil solution concentrations of mentioned uranium species.
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.
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.
238U-Series in Fe Oxy/Hydroxides by LA-MC-ICP-MS, New Insights Into Weathering Geochronology
NASA Astrophysics Data System (ADS)
Bernal, J.; McCulloch, M.; Eggins, S.; Grun, R.; Eggleton, R.
2003-12-01
The establishment of a geochronological framework for weathering processes is essential for an understanding of the evolution of the regolith and its dynamics. However, there are few robust answers regarding the absolute age of weathering and its rates. Nowadays, 40Ar/39Ar analysis of Mn-Oxides (cryptomelane) and K-bearing secondary sulphates have provided one of the few generally reliable chronometers (e.g. 1), but is restricted to high-K secondary phases. This work presents a different approach to obtain geochronological information from weathering minerals, namely measurement of 238U-series disequilibria in authigenic Fe oxy/hydroxides. These may be potentially useful recorders of weathering processes as they commonly occur as weathering products and have high affinity towards dissolved uranyl complexes. Furthermore, U-Th fractionation during weathering has been extensively reported [2], effectively resetting the U/230Th geochronometer. LA-MC-ICP-MS facilitates in situ measurement of 238U-series disequilibria in authigenic microcrystalline iron oxy/hydroxides (precipitated between cracks and veins in partially and heavily weathered chlorite-muscovite schist) and pisoliths (ferruginous concretions). Contrary to previous studies [e.g. 3], in situ measurement of 238U-nuclides enables selective analysis or iron oxy/hydroxides phases, minimizes contributions from allogenic phases and, reduces the need of mathematical corrections to obtain the activity ratios for the authigenic phase [4, 5]. The results suggest that supergene iron oxy/hydroxides are good recorders of weathering processes; they precipitate during the early stages of weathering, reflect the U-isotopic composition of the groundwater, appear to act as closed-systems in weathering conservative environments, and behave in a predictable fashion when subjected to intense weathering and leaching conditions. The 230Th-ages of the iron oxy/hydroxides indicate that the timing and intensity of weathering appears to be largely controlled by global climatic changes, suggesting that weathering rates have not been constant during the last 300 ka in Northern Australia. References: 1 P.M. Vasconcelos. Annual Review in Earth and Planetary Sciences 27(1), 183-229, (1999) 2 M. Ivanovich and R.S. Harmon, Uranium-series disequilibrium : applications to earth, marine, and environmental science, xxxiv, 910 pp., Oxford University Press, Oxford, (1992) 3 S.A. Short, R.T. Lowson, J. Ellis and D.M. Price. Geochimica et Cosmochimica Acta 53, 1379-1389, (1989) 4 K.R. Ludwig and D.M. Titterington. Geochimica et Cosmochimica Acta 58(22), 5031-5042, (1994) 5 Luo, S. and T. L. Ku. Geochimica et Cosmochimica Acta 55(2): 555-564. (1991)
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
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
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.
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.
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).
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
Isotopic analysis of uranium in natural waters by alpha spectrometry
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.
Radioactivity of Consumer Products
NASA Astrophysics Data System (ADS)
Peterson, David; Jokisch, Derek; Fulmer, Philip
2006-11-01
A variety of consumer products and household items contain varying amounts of radioactivity. Examples of these items include: FiestaWare and similar glazed china, salt substitute, bananas, brazil nuts, lantern mantles, smoke detectors and depression glass. Many of these items contain natural sources of radioactivity such as Uranium, Thorium, Radium and Potassium. A few contain man-made sources like Americium. This presentation will detail the sources and relative radioactivity of these items (including demonstrations). Further, measurements of the isotopic ratios of Uranium-235 and Uranium-238 in several pieces of china will be compared to historical uses of natural and depleted Uranium. Finally, the presenters will discuss radiation safety as it pertains to the use of these items.
In-situ, time resolved monitoring of uranium in BFS:OPC grout. Part 2: Corrosion in water.
Stitt, C A; Paraskevoulakos, C; Banos, A; Harker, N J; Hallam, K R; Pullin, H; Davenport, A; Street, S; Scott, T B
2018-06-18
To reflect potential conditions in a geological disposal facility, uranium was encapsulated in grout and submersed in de-ionised water for time periods between 2-47 weeks. Synchrotron X-ray Powder Diffraction and X-ray Tomography were used to identify the dominant corrosion products and measure their dimensions. Uranium dioxide was observed as the dominant corrosion product and time dependent thickness measurements were used to calculate oxidation rates. The effectiveness of physical and chemical grout properties to uranium corrosion and mobilisation is discussed and Inductively Coupled Plasma Mass Spectrometry was used to measure 238 U (aq) content in the residual water of several samples.
NASA Astrophysics Data System (ADS)
Krawczynski, M.; McLean, N.
2017-12-01
One of the most accurate and useful ways of determining the age of rocks that formed more than about 500,000 years ago is uranium-lead (U-Pb) geochronology. Earth scientists use U-Pb geochronology to put together the geologic history of entire regions and of specific events, like the mass extinction of all non-avian dinosaurs about 66 million years ago or the catastrophic eruptions of supervolcanoes like the one currently centered at Yellowstone. The mineral zircon is often utilized because it is abundant, durable, and readily incorporates uranium into its crystal structure. But it excludes thorium, whose isotope 230Th is part of the naturally occurring isotopic decay chain from 238U to 206Pb. Calculating a date from the relative abundances of 206Pb and 238U therefore requires a correction for the missing 230Th. Existing experimental and observational constraints on the way U and Th behave when zircon crystallizes from a melt are not known precisely enough, and thus currently the uncertainty in dates introduced by they `Th correction' is one of the largest sources of systematic error in determining dates. Here we present preliminary results on our study of actinide partitioning between zircon and melt. Experiments have been conducted to grow zircon from melts doped with U and Th that mimic natural magmas at a range of temperatures, and compositions. Synthetic zircons are separated from their coexisting glass and using high precision and high-spatial-resolution techniques, the abundance and distribution of U and Th in each phase is determined. These preliminary experiments are the beginning of a study that will result in precise determination of the zircon/melt uranium and thorium partition coefficients under a wide variety of naturally occurring conditions. This data will be fit to a multidimensional surface using maximum likelihood regression techniques, so that the ratio of partition coefficients can be calculated for any set of known parameters. The results of this study will reduce the largest source of uncertainty in dating young zircons and improve the accuracy of U-Pb dates, improving our ability to tell time during geologic processes. The attainment of more accurate timing of the geologic timescale is important to geologists of all disciplines, from paleontology to planetary cosmochemistry to geobiology.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Thomas, P.A.; Sheard, J.W.; Swanson, S.
1994-12-31
This report examines baseline concentrations and transfer of the uranium decay products polonium-210 and lead-210 in the lichen-caribou-wolf food chain at two locations in the Northwest Territories, Baker Lake and Snowdrift. At each location, concentrations of the two radionuclides were determined in the lichen species Cetraria nivalis and Cladina mitis, and several tissues from caribou and wolves. Baseline concentrations and transfer coefficients within the food chain were compared between the two locations. Lichen samples were also collected from Kasba Lake, a third hunting ground used by northern Saskatchewan hunters. The lichen species chosen were common forage for caribou. Both themore » predominant lichen species at each location and rumen contents were used to estimate the winter diet of caribou in the calculation of transfer coefficients. The results are relevant to environmental monitoring in areas of potential future uranium mining development and the transfer coefficients determined in the study may be used to estimate radionuclide concentrations and radiation doses in future environmental assessments.« less
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.
Dlamini, S G; Mathuthu, M M; Tshivhase, V M
2016-03-01
High concentrations of radionuclides and toxic elements in gold mine tailings facilities present a health hazard to the environment and people living near that area. Soil and water samples from selected areas around the Princess Mine dump were collected. Soil sampling was done on the surface (15 cm) and also 100 cm below the surface. Water samples were taken from near the dump, mid-stream and the flowing part of the stream (drainage pipe) passing through Roodepoort from the mine dump. Soil samples were analyzed by gamma-ray spectroscopy using a HPGe detector to determine the activity concentrations of (238)U, (232)Th and (4) (40)K from the activities of the daughter nuclides in the respective decay chains. The average activity concentrations for uranium and thorium in soil were calculated to be 129 ± 36.1 Bq/kg and 18.1 ± 4.01 Bq/kg, respectively. Water samples were analyzed using Inductively Coupled Plasma Mass Spectrometer. Transfer factors for uranium and thorium from soil to water (at point A closest to dump) were calculated to be 0.494 and 0.039, respectively. At point Z2, which is furthest from the dump, they were calculated to be 0.121 and 0.004, respectively. These transfer factors indicate that there is less translocation of the radionuclides as the water flows. Copyright © 2016 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mujaini, M., E-mail: madihah@uniten.edu.my; Chankow, N.; Yusoff, M. Z.
2016-01-22
Uranium ore can be easily detected due to various gamma-ray energies emitted from uranium daughters particularly from {sup 238}U daughters such as {sup 214}Bi, {sup 214}Pb and {sup 226}Ra. After uranium is extracted from uranium ore, only low energy gamma-rays emitted from {sup 235}U may be detected if the detector is placed in close contact to the specimen. In this research, identification and characterization of uranium bearing materials is experimentally investigated using direct measurement of gamma-rays from {sup 235}U in combination with the x-ray fluorescence (XRF) technique. Measurement of gamma-rays can be conducted by using high purity germanium (HPGe) detectormore » or cadmium telluride (CdTe) detector while a {sup 57}Coradioisotope-excited XRF spectrometer using CdTe detector is used for elemental analysis. The proposed technique was tested with various uranium bearing specimens containing natural, depleted and enriched uranium in both metallic and powder forms.« less
206Pb-230Th-234U-238U and 207Pb-235U geochronology of Quaternary opal, Yucca Mountain, Nevada
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.
NASA Astrophysics Data System (ADS)
Wuenschel, S.; Hagel, K.; Barbui, M.; Gauthier, J.; Cao, X. G.; Wada, R.; Kim, E. J.; Majka, Z.; Płaneta, R.; Sosin, Z.; Wieloch, A.; Zelga, K.; Kowalski, S.; Schmidt, K.; Ma, C.; Zhang, G.; Natowitz, J. B.
2018-06-01
The production of α -particle decaying heavy nuclei in reactions of 7.5-6.1 MeV/nucleon 238U +232Th was explored using an in-beam detection array composed of YAP scintillators and gas ionization chamber-Si telescopes. Comparisons of α energies and half-lives for the observed products with those of the previously known isotopes and with theoretically predicted values indicate the observation of a number of previously unreported α emitters. α -particle decay energies reaching as high as 12 MeV are observed. Many of these are expected to be from decay of previously unseen relatively neutron rich products. While the contributions of isomeric states require further exploration and specific isotope identifications need to be made, the production of heavy isotopes with quite high atomic numbers is suggested by the data.
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
Parrish, Randall R; Thirlwall, Matthew F; Pickford, Chris; Horstwood, Matthew; Gerdes, Axel; Anderson, James; Coggon, David
2006-02-01
Accidental exposure to depleted or enriched uranium may occur in a variety of circumstances. There is a need to quantify such exposure, with the possibility that the testing may post-date exposure by months or years. Therefore, it is important to develop a very sensitive test to measure precisely the isotopic composition of uranium in urine at low levels of concentration. The results of an interlaboratory comparison using sector field (SF)-inductively coupled plasma-mass spectrometry (ICP-MS) and multiple collector (MC)-ICP-MS for the measurement of uranium concentration and U/U and U/U isotopic ratios of human urine samples are presented. Three urine samples were verified to contain uranium at 1-5 ng L and shown to have natural uranium isotopic composition. Portions of these urine batches were doped with depleted uranium (DU) containing small quantities of U, and the solutions were split into 100 mL and 400 mL aliquots that were subsequently measured blind by three laboratories. All methods investigated were able to measure accurately U/U with precisions of approximately 0.5% to approximately 4%, but only selected MC-ICP-MS methods were capable of consistently analyzing U/U to reasonable precision at the approximately 20 fg L level of U abundance. Isotope dilution using a U tracer demonstrates the ability to measure concentrations to better than +/-4% with the MC-ICP-MS method, though sample heterogeneity in urine samples was shown to be problematic in some cases. MC-ICP-MS outperformed SF-ICP-MS methods, as was expected. The MC-ICP-MS methodology described is capable of measuring to approximately 1% precision the U/U of any sample of human urine over the entire range of uranium abundance down to <1 ng L, and detecting very small amounts of DU contained therein.
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.
Uranium-234 anomalies in corals older than 150,000 years
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bard, E.; Fairbanks, R.G.; Zindler, A.
1991-08-01
The authors present new precise U-Th ages of well-preserved coral specimens collected from the island of Barbados, West Indies, and the atoll of Mururoa, French Polynesia. Their new data confirm the ages attributed to oxygen isotope stage 7 in the framework of the Milankovitch theory. By using thermal ionization mass spectrometry (TIMS), it is also possible to quantify precisely the [sup 234]U/[sup 238]U ratios in corals. Samples older than 150 kyr B.P. are shown to be characterized by significant excesses of [sup 234]U relative to the uranium isotopic composition expected if the corals grew in present-day sea water. Assuming thatmore » the [sup 230]Th-ingrowth ages are accurate, these anomalies translate into high initial [sup 234]U/[sup 238]U ratios: about 1.2 at 200 kyr and up to 1.5 at about 450 kyr B.P. They propose that the anomalies result from both diagenetic addition and replacement of U and possibly from global changes in the [sup 234]U/[sup 238]U composition of the sea water through time. The [sup 234]U anomalies cast doubt on the accuracy of the classical [sup 230]Th-ingrowth dating method in old corals, and in particular for the use of measured [sup 234]U/[sup 238]U ratios alone to date corals older than 150 kyr.« less
Comprehensive Evaluation of Soil Near Uranium Tailings, Beishan City, China.
Xun, Yan; Zhang, Xinjia; Chaoliang, Chen; Luo, Xuegang; Zhang, Yu
2018-06-01
To evaluate the impact of uranium tailings on soil composition and soil microbial, six soil samples at different distance from the uranium tailings (Beishan City, China) were collected for further analysis. Concentrations of radionuclides ( 238 U and 232 Th), heavy metals (Mn, Cd, Cr, Ni, Zn, and Pb) and organochlorine pesticide were determined by ICP-MS and GC, they were significantly higher than those of the control. And the Average Well Color Development as well as the Shannon, the Evenness, and the Simpson index were calculated to evaluate the soil microbial diversity. The carbon utilization model of soil microbial community was also analyzed by Biolog-eco. All results indicated that uranium tailings leaded to excessive radionuclides and heavy metals, and decreased the diversity of the soil microbial community. Our study will provide a valuable basis for soil quality evaluation around uranium tailing repositories and lay a foundation for the management and recovery of uranium tailings.
Analysis of solid uranium samples using a small mass spectrometer
NASA Astrophysics Data System (ADS)
Kahr, Michael S.; Abney, Kent D.; Olivares, José A.
2001-07-01
A mass spectrometer for isotopic analysis of solid uranium samples has been constructed and evaluated. This system employs the fluorinating agent chlorine trifluoride (ClF 3) to convert solid uranium samples into their volatile uranium hexafluorides (UF 6). The majority of unwanted gaseous byproducts and remaining ClF 3 are removed from the sample vessel by condensing the UF 6 and then pumping away the unwanted gases. The UF 6 gas is then introduced into a quadrupole mass spectrometer and ionized by electron impact ionization. The doubly charged bare metal uranium ion (U 2+) is used to determine the U 235/U 238 isotopic ratio. Precision and accuracy for several isotopic standards were found to be better than 12%, without further calibration of the system. The analysis can be completed in 25 min from sample loading, to UF 6 reaction, to mass spectral analysis. The method is amenable to uranium solid matrices, and other actinides.
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.
Bland, D; Rona, R; Coggon, D; Anderson, J; Greenberg, N; Hull, L; Wessely, S
2007-01-01
Objectives To assess the distribution and risk factors of depleted uranium uptake in military personnel who had taken part in the invasion of Iraq in 2003. Methods Sector field inductively coupled plasma-mass spectrometry (SF-ICP-MS) was used to determine the uranium concentration and 238U/235U isotopic ratio in spot urine samples. The authors collected urine samples from four groups identified a priori as having different potential for exposure to depleted uranium. These groups were: combat personnel (n = 199); non-combat personnel (n = 96); medical personnel (n = 22); and “clean-up” personnel (n = 24) who had been involved in the maintenance, repair or clearance of potentially contaminated vehicles in Iraq. A short questionnaire was used to ascertain individual experience of circumstances in which depleted uranium exposure might have occurred. Results There was no statistically significant difference in the 238U/235U ratio between groups. Mean ratios by group varied from 138.0 (95% CI 137.3 to 138.7) for clean-up personnel to 138.2 (95% CI 138.0 to 138.5) for combat personnel, and were close to the ratio of 137.9 for natural uranium. The two highest individual ratios (146.9 and 147.7) were retested using more accurate, multiple collector inductively coupled plasma-mass spectrometry (MC-ICP-MS) and found to be within measurement of error of that for natural uranium. There were no significant differences in isotope ratio between participants according to self-reported circumstances of potential depleted uranium exposure. Conclusions Based on measurements using a SF-ICP-MS apparatus, this study provides reassurance following concern for potential widespread depleted uranium uptake in the UK military. The rare occurrence of elevated ratios may reflect the limits of accuracy of the SF-ICP-MS apparatus and not a real increase from the natural proportions of the isotopes. Any uptake of depleted uranium among participants in this study sample would be very unlikely to have any implications for health. PMID:17609224
ENDF/B-VII.0: Next Generation Evaluated Nuclear Data Library for Nuclear Science and Technology
NASA Astrophysics Data System (ADS)
Chadwick, M. B.; Obložinský, P.; Herman, M.; Greene, N. M.; McKnight, R. D.; Smith, D. L.; Young, P. G.; MacFarlane, R. E.; Hale, G. M.; Frankle, S. C.; Kahler, A. C.; Kawano, T.; Little, R. C.; Madland, D. G.; Moller, P.; Mosteller, R. D.; Page, P. R.; Talou, P.; Trellue, H.; White, M. C.; Wilson, W. B.; Arcilla, R.; Dunford, C. L.; Mughabghab, S. F.; Pritychenko, B.; Rochman, D.; Sonzogni, A. A.; Lubitz, C. R.; Trumbull, T. H.; Weinman, J. P.; Brown, D. A.; Cullen, D. E.; Heinrichs, D. P.; McNabb, D. P.; Derrien, H.; Dunn, M. E.; Larson, N. M.; Leal, L. C.; Carlson, A. D.; Block, R. C.; Briggs, J. B.; Cheng, E. T.; Huria, H. C.; Zerkle, M. L.; Kozier, K. S.; Courcelle, A.; Pronyaev, V.; van der Marck, S. C.
2006-12-01
We describe the next generation general purpose Evaluated Nuclear Data File, ENDF/B-VII.0, of recommended nuclear data for advanced nuclear science and technology applications. The library, released by the U.S. Cross Section Evaluation Working Group (CSEWG) in December 2006, contains data primarily for reactions with incident neutrons, protons, and photons on almost 400 isotopes, based on experimental data and theory predictions. The principal advances over the previous ENDF/B-VI library are the following: (1) New cross sections for U, Pu, Th, Np and Am actinide isotopes, with improved performance in integral validation criticality and neutron transmission benchmark tests; (2) More precise standard cross sections for neutron reactions on H, 6Li, 10B, Au and for 235,238U fission, developed by a collaboration with the IAEA and the OECD/NEA Working Party on Evaluation Cooperation (WPEC); (3) Improved thermal neutron scattering; (4) An extensive set of neutron cross sections on fission products developed through a WPEC collaboration; (5) A large suite of photonuclear reactions; (6) Extension of many neutron- and proton-induced evaluations up to 150 MeV; (7) Many new light nucleus neutron and proton reactions; (8) Post-fission beta-delayed photon decay spectra; (9) New radioactive decay data; (10) New methods for uncertainties and covariances, together with covariance evaluations for some sample cases; and (11) New actinide fission energy deposition. The paper provides an overview of this library, consisting of 14 sublibraries in the same ENDF-6 format as the earlier ENDF/B-VI library. We describe each of the 14 sublibraries, focusing on neutron reactions. Extensive validation, using radiation transport codes to simulate measured critical assemblies, show major improvements: (a) The long-standing underprediction of low enriched uranium thermal assemblies is removed; (b) The 238U and 208Pb reflector biases in fast systems are largely removed; (c) ENDF/B-VI.8 good agreement for simulations of thermal high-enriched uranium assemblies is preserved; (d) The underprediction of fast criticality of 233,235U and 239Pu assemblies is removed; and (e) The intermediate spectrum critical assemblies are predicted more accurately. We anticipate that the new library will play an important role in nuclear technology applications, including transport simulations supporting national security, nonproliferation, advanced reactor and fuel cycle concepts, criticality safety, fusion, medicine, space applications, nuclear astrophysics, and nuclear physics facility design. The ENDF/B-VII.0 library is archived at the National Nuclear Data Center, BNL, and can be retrieved from www.nndc.bnl.gov.
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.
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
(238)U and total radioactivity in drinking waters in Van province, Turkey.
Selçuk Zorer, Özlem; Dağ, Beşir
2014-06-01
As part of the national survey to evaluate natural radioactivity in the environment, concentration levels of total radioactivity and natural uranium have been analysed in drinking water samples. A survey to study natural radioactivity in drinking waters was carried out in the Van province, East Turkey. Twenty-three samples of drinking water were collected in the Van province and analysed for total α, total β and (238)U activity. The total α and total β activities were counted by using the α/β counter of the multi-detector low background system (PIC MPC-9604), and the (238)U concentrations were determined by inductively coupled plasma-mass spectrometry (Thermo Scientific Element 2). The samples were categorised according to origin: tap, spring or mineral supply. The activity concentrations for total α were found to range from 0.002 to 0.030 Bq L(-1) and for total β from 0.023 to 1.351 Bq L(-1). Uranium concentrations ranging from 0.562 to 14.710 μg L(-1) were observed in drinking waters. Following the World Health Organisation rules, all investigated waters can be used as drinking water.
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
Nuclear stopping and collective flow in CSR/LanZhou energy region
NASA Astrophysics Data System (ADS)
Luo, X.-F.; Dong, X.; Shao, M.; Li, C.; Chen, H.-F.; Wu, K.-J.; Xu, H.-S.
2011-06-01
Nuclear stopping and collective flow for two pairs of symmetric colliding nuclei: 238U+238U and 129Xe+129Xe, which are proposed to be accelerated on Cooling Storage Ring (CSR), External Target Facility (ETF), LanZhou, China, are studied by a hadronic transport model ART1.0. The incident beam energy of Uranium and Xenon can be delivered up to 520 MeV/nucleon and 900MeV/nucleon, respectively. At this CSR energy region, the hot, dense nuclear matter are thought to be obtained in the lab, which is an idea circumstance to study the nuclear equation of state (EoS). As deformation of the Uranium nuclei, it is predicted that significant large baryon density in the tip-tip U+U collision patterns and the large elliptic flow in body-body collision pattern are both avail to study the nuclear EoS.
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
HAGRID/ VANDLE spectroscopy of Rb decays
NASA Astrophysics Data System (ADS)
King, Thomas; Grzywacz, Robert; Taylor, Steven; Paulauskas, Stanley; Smith, Karl; Vandle Collaboration
2017-09-01
Many neutron-rich isotopes that contribute in both decay heat production and r-process nucleosynthesis have substantial beta-delayed neutron branching ratios. Beta-delayed neutron emission is a relatively complicated mechanism which can leave the daughter in an gamma-emitting excited state. A comprehensive understanding of their energy output and decay strength, S_beta, therefore requires the detection of both neutrons and gamma rays in coincidence. A series of measurements of delayed neutron precursors were performed at the On-Line Test Facility (OLTF) at the Oak Ridge National Laboratories using chemically selective ion sources and an enhanced VANDLE array. The main goal of this experiment was to revisit the decays of IAEA-marked priority precursors, including bromine, rubidium, cesium, and iodine, that are required to model the global properties in the fission of 238U.The unique data set, with neutron and gamma ray coincidences, benefited from the addition of a high-efficiency gamma-ray array, consisting of 16 LaBr3 crystals (HAGRiD), and a set of large volume NaI detectors to the VANDLE array. Characterization of and preliminary results from the new gamma-ray array for the decays of 94Rb and 97Rb will be presented. National Nuclear Security Administration under the Stewardship Science Academic Alliances program through DOE Award No. DE-NA0002132 and the Office of Nuclear Physics, U.S. Department of Energy under Award No. DE-FG02-96ER40983.
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.
Lawrence, E.; Poeter, E.; Wanty, R.
1991-01-01
Integrated studies of geohydrology, geochemistry, and geology of crystalline rocks in the vicinity of Conifer, Colorado, reveal that radon concentrations do not correlate with variations in concentrations of other dissolved species. Concentrations of major ions show systematic variations along selected groundwater flowpaths, whereas radon concentrations are dependent on local geochemical and geologic phenomena (such as localized uranium concentration in the rock or the presence of faults or folds). When radon enters the flow system, concentrations do not increase along flowpaths because its decay rate is fast relative to groundwater flow rates. Radon-222 is not in secular equilibrium with 238U and 226Ra in the water. Therefore, most of the 238U and 226Ra necessary to support the waterborne 222Rn must be present locally in the rock. High concentrations of dissolved radon are not found in zones of high transmissivity, and transmissivity is not correlated with rock type in the study area. A higher transmissivity can be indicative of higher water-volume to rock-surface-area ratios, which could effectively dilute 222Rn entering the water and/or may indicate that emanated radon is carried away more rapidly. Water samples collected from individual wells over periods of several months showed significant fluctuations in the dissolved 222Rn content. This fluctuation may be controlled by changes in the contributions of water-producing zones within the well resulting from seasonal fluctuations of the water table and/or pumping stresses. ?? 1991.
Progress on 241Am Production for Use in Radioisotope Power Systems
NASA Astrophysics Data System (ADS)
Baker, S. R.; Bell, K. J.; Brown, J.; Carrigan, C.; Carrott, M. J.; Gregson, C.; Clough, M.; Maher, C. J.; Mason, C.; Rhodes, C. J.; Rice, T. G.; Sarsfield, M. J.; Stephenson, K.; Taylor, R. J.; Tinsley, T. P.; Woodhead, D. A.; Wiss, T.
2014-08-01
Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. Power sources generate electricity from the thermal energy from alpha decay of the radioisotope 238Pu via thermo-electric conversion. Production of 238Pu requires specialist facilities including a nuclear reactor and reprocessing plants that are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is a feasible alternative to 238Pu that can provide a heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). As a daughter product of 241Pu decay, 241Am is present at 1000s kg levels within the UK civil plutonium stockpile.A chemical separation process is required to extract the 241Am in a pure form and this paper describes such a process, successfully developed to the proof of concept stage.
Introduction to Pits and Weapons Systems (U)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Kautz, D.
2012-07-02
A Nuclear Explosive Package includes the Primary, Secondary, Radiation Case and related components. This is the part of the weapon that produces nuclear yield and it converts mechanical energy into nuclear energy. The pit is composed of materials that allow mechanical energy to be converted to electromagnetic energy. Fabrication processes used are typical of any metal fabrication facility: casting, forming, machining and welding. Some of the materials used in pits include: Plutonium, Uranium, Stainless Steel, Beryllium, Titanium, and Aluminum. Gloveboxes are used for three reasons: (1) Protect workers and public from easily transported, finely divided plutonium oxides - (a) Plutoniummore » is very reactive and produces very fine particulate oxides, (b) While not the 'Most dangerous material in the world' of Manhattan Project lore, plutonium is hazardous to health of workers if not properly controlled; (2) Protect plutonium from reactive materials - (a) Plutonium is extremely reactive at ambient conditions with several components found in air: oxygen, water, hydrogen, (b) As with most reactive metals, reactions with these materials may be violent and difficult to control, (c) As with most fabricated metal products, corrosion may significantly affect the mechanical, chemical, and physical properties of the product; and (3) Provide shielding from radioactive decay products: {alpha}, {gamma}, and {eta} are commonly associated with plutonium decay, as well as highly radioactive materials such as {sup 241}Am and {sup 238}Pu.« less
Isotopic evidence for reductive immobilization of uranium across a roll-front mineral deposit
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
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.
NASA Astrophysics Data System (ADS)
Ma, Lin
2015-04-01
Lin Ma1, Yvette Pereyra1, Peter B Sak2, Jerome Gaillardet3, Heather L Buss4 and Susan L Brantley5, (1) University of Texas at El Paso, El Paso, TX, United States, (2) Dickinson College, Carlisle, PA, United States, (3) Institute de Physique d Globe Paris, Paris, France, (4) University of Bristol, Bristol, United Kingdom, (5) Pennsylvania State University Main Campus, University Park, PA, United States Uranium-series isotopes fractionate during chemical weathering and their activity ratios can be used to determine timescales and rates of soil formation. Such soil formation rates provide important information to understand processes related to rapid soil formation in tropical volcanic settings, especially with respect to their fertility and erosion. Recent studies also highlighted the use of U-series isotopes to trace and quantify atmospheric inputs to surface soils. Such a process is particularly important in providing mineral nutrients to ecosystems in highly depleted soil systems such as the tropical soils. Here, we report U-series isotope compositions in thick soil profiles (>10 m) developed on andesitic pyroclastic flows in Basse-Terre Island of French Guadeloupe. Field observations have shown heterogeneity in color and texture in these thick profiles. However, major element chemistry and mineralogy show some general depth trends. The main minerals present throughout the soil profile are halloysite and gibbsite. Chemically immobile elements such as Al, Fe, and Ti show a depletion profile relative to Th while elements such as K, Mn, and Si show a partial depletion profile at depth. Mobile elements such as Ca, Mg, and Sr have undergone intensive weathering at depths, and an addition profile near the surface, most likely related to atmospheric inputs. (238U/232Th) activity ratios in one soil profile from the Brad David watershed in this study ranged from 0.374 to 1.696, while the (230Th/232Th) ratios ranged from 0.367 to 1.701. A decrease of (238U/232Th) in the deep soil profile depth is observed, and then an increase to the surface. The (230Th /232Th) ratios showed a similar trend as (238U/232Th). Marine aerosols and atmospheric dust from the Sahara region are most likely responsible for the addition of U in shallow soils. Intensive chemical weathering is responsible for the loss of U at depth, consistent with these observations of major element chemistry and mineralogy. Furthermore, U-series chemical weathering model suggests that the weathering duration from 12m to 4m depth in this profile is about 250kyr, with a weathering advancing rate of ~30 m/Ma. The rate is also about one order of magnitude lower than the weathering rate (~300 m/Ma) determined by river chemistry for this watershed. In this profile, the augered core didn't reach the unweathered bedrock. Hence, the derived slow weathering rate most likely represents the intensive weathering of clay minerals, while the transformation of fresh bedrock to regolith occurs at much great depth beneath the thick regolith. The marine aerosols and atmospheric dust are important sources of mineral nutrients for highly depleted surface soils.
Tables for determining lead, uranium, and thorium isotope ages
NASA Technical Reports Server (NTRS)
Schonfeld, E.
1974-01-01
Tables for determining lead, uranium, and thorium isotope ages are presented in the form of computer printouts. Decay constants, analytical expressions for the functions evaluated, and the precision of the calculations are briefly discussed.
Clewett, G.H.; Lee, DeW.A.
1958-05-20
A new method is described for isotopic enrichment of uranium. It has been found that when an aqueous acidic solution of ionic tetravalent uraniunn is contacted with chelate complexed tetravalent uranium, the U/sup 238/ preferentially concentrates in the complexed phase while U/sup 235/ concentrates in the ionic phase. The effect is enhanced when the chelate compound is water insoluble and is dissolved in a water-immiscible organic solvent. Cupferron is one of a number of sultable complexing agents, and chloroform is a suitable organic solvent.
TOF-SIMS for Rapid Nuclear Forensics Evaluation of Uranium Oxide Particles
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
NASA Astrophysics Data System (ADS)
Sampalmieri, G.; Iadanza, A.; Cipollari, P.; Cosentino, D.; Lo Mastro, S.
2009-04-01
Bottom redox conditions in marine and lacustrine ancient basins are often inferred by the occurrence of peculiar sedimentological structures and microfaunal assemblages. The co-occurrence, in such environments, of authigenic uranium, framboidal pyrite, barite and Fe-Mn nodules and encrustations, provides a good constraint for palaeo reconstructions. Authigenic uranium is a common constituent of hydrocarbon source rocks: it forms at the sediment-water interface under oxygen-deficient conditions and accumulates together with organic matter (OM). Its precipitation is triggered by the reduction of the soluble U6+ion in seawater to insoluble U4+. With respect to black shales, uranium content has even been used to estimate the TOC. Also authigenic pyrite forms under anoxic conditions and replaces organic matter: 1) the increase in pyrite content and in organic matter are directly correlated; 2) the size distribution of framboidal pyrite (consistent with sulphate-reducing bacterial activity) is considered a measure of redox conditions within the sediment. Barite is an authigenic mineral related to Corg content, since its organic precipitation is triggered by sulphate-reduction processes occurring in decaying OM-bearing microenvironments. Finally, also Fe-Mn oxyhydroxide are typical indicators of redox conditions. About 6 My ago the Mediterranean Sea underwent a giant event of concentration referred to as Messinian Salinity Crisis, which can be roughly subdivided into an evaporitic and a post evaporitic phase. The post evaporitic phase (p-ev; 5.61-5.33 Ma) developed in a context of humid conditions and can be further distinguished into two steps: p-ev1 (early post evaporitic phase) and p-ev2 (late post evaporitic phase). Previous works focused on pev2, which is interpreted to represent the establishment of brackish water conditions (Lago-Mare biofacies). In other respects, the palaeoenvironment of p-ev1 deposits, mostly represented by resedimented evaporitic deposits or barren laminated sediments, hasn't been thoroughly clarified yet. The aim of the present study, dealing with messinian p-ev1 deposits from Marche and Maiella successions, is to provide more details in the definition of the environment developed during the early post-evaporitic phase. Since the lamination and the absence of benthic fauna suggest the occurrence of anoxic conditions, the following indirect proxies for the detection of organic matter have been investigated: 1) sedimentary fabric and microfacies; 2) framboidal pyrite size distribution; 3) natural radioactivity (authigenic uranium values, Th/U ratios). Natural radioactivity has been achieved through gamma spectrometry, with field and laboratory specific techniques. In the Maccarone section (Marche region), p-ev1 deposits are constituted by: barren greyish shales; laminated black shales interbedded with calcitic and ankeritic horizons; thin intercalations of sandstones. Organic-matter and framboidal pyrite commonly occur. Size analysis of framboids populations yielded a mean diameter of 4÷8 m, typical of disaerobic facies. Microfacies analysis yielded also the presence of crystals aggregates of barite, up to 50 m in size, and of isolated detrital (silicilastic) crystals. Without considering γ-ray values of the volcaniclastic layer (52-65 Cps) occurring within the p-ev1 interval, black shales horizons revealed the maximum natural radioactivity (NRD of about 50 Cps) recorded inthe studied section. Lower γ-activity characterizes the calcitic layers (i.e. "Colombacci") and the ankerites. Field NRD spectra acquired on different lithologies, showed variable contributions of 238U, 232Th and 40K. Both the blue-greyish shales and the black shales are characterized by total NRD related to the three main radioelements: 40K is associated to abundant 238U content (Thppm/Uppm 1). The 238U content is primarily referable to processes of organic matter enrichment (authigenic uranium) and secondarily to the input of detrital grains. In contrast, 40K and 232Th are entirely ascribed to the clastic fraction. P-ev1 deposits from Maiella section consist of thinly-laminated grey-brownish pelites, enclosing carbonatic lenses and interrupted horizons. The pelitic fraction contains Fe-Mn-Ni encrustated micronodules. The carbonate portion is made up of locally brecciated calcitic limestones, associated with calcitic concretions and discontinuous laminae. Traces of organic matter and bitumen have been observed in thin section. Framboidal pyrite occurs both as single element and as aggregate, reaching dimensions up to about 10 m. Barite and celestite occur as well. NRD measurements yielded high values of radioactivity both in carbonates (20-63 Cps) and in terrigenous sediments (21-70 Cps). Limestones NRD-spectra showed a 238U-dominant (5 ppm in content) radioactivity. 238U is totally referable to an authigenic origin, since the γ-activity of limestones is devoid of contributions from 40K and 232Th (proxies for the detritic fraction). In the latest Messinian frame, authigenic uranium, barite, ankerite, Fe-Mn oxyhydroxide and framboidal pyrite indicate strongly palaeoredox conditions (from disaerobic to fully anoxic). In particular, with respect to NRD data, this peculiar environment is confirmed by the Th/U ratio, mostly
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.
The natural radioactivity in some Nigerian foodstuffs
NASA Astrophysics Data System (ADS)
Olomo, James B.
1990-12-01
The average activity concentrations of seven locally produced food commodities that form the total diets of a baby, a teenager or an adult male in Nigeria were measured by means of a well-calibrated high-resolution lithium-drifted germanium (Ge(Li)) spectrometer system. The food commodities were collected at several centers such as a nuclear research center as well as metropolitan and industrial areas. The emission lines identified with reliable regularity belonged to the 238U and 232Th decay series. The other isotope is a non-related naturally occurring radionuclide, 40K. Average total specific-activity values of 7.29 ± 1.08, 6.27 ± 1.01 and 11.23 ± 1.64 Bq/kg for 238U, 232Th and 40K, respectively, were obtained for the seven food commodities studied. The food samples were also checked for fission-product residues ( 137Cs and 90Sr) from atmospheric weapons tests which are slowly being purged from the food chain. Their estimation revealed that they were below the minimum detectable limit determined at a two-standard deviation analytical error.
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
Fluxes of 238U decay series radionuclides in a dicalcium phosphate industrial plant.
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.
NASA Astrophysics Data System (ADS)
De Vleeschouwer, David; Dunlea, Ann G.; Auer, Gerald; Anderson, Chloe H.; Brumsack, Hans; de Loach, Aaron; Gurnis, Michael; Huh, Youngsook; Ishiwa, Takeshige; Jang, Kwangchul; Kominz, Michelle A.; März, Christian; Schnetger, Bernhard; Murray, Richard W.; Pälike, Heiko
2017-03-01
During International Ocean Discovery Program (IODP) expeditions, shipboard-generated data provide the first insights into the cored sequences. The natural gamma radiation (NGR) of the recovered material, for example, is routinely measured on the ocean drilling research vessel DV JOIDES Resolution. At present, only total NGR counts are readily available as shipboard data, although full NGR spectra (counts as a function of gamma-ray energy level) are produced and archived. These spectra contain unexploited information, as one can estimate the sedimentary contents of potassium (K), thorium (Th), and uranium (U) from the characteristic gamma-ray energies of isotopes in the 40K, 232Th, and 238U radioactive decay series. Dunlea et al. (2013) quantified K, Th, and U contents in sediment from the South Pacific Gyre by integrating counts over specific energy levels of the NGR spectrum. However, the algorithm used in their study is unavailable to the wider scientific community due to commercial proprietary reasons. Here, we present a new MATLAB algorithm for the quantification of NGR spectra that is transparent and accessible to future NGR users. We demonstrate the algorithm's performance by comparing its results to shore-based inductively coupled plasma-mass spectrometry (ICP-MS), inductively coupled plasma-emission spectrometry (ICP-ES), and quantitative wavelength-dispersive X-ray fluorescence (XRF) analyses. Samples for these comparisons come from eleven sites (U1341, U1343, U1366-U1369, U1414, U1428-U1430, and U1463) cored in two oceans during five expeditions. In short, our algorithm rapidly produces detailed high-quality information on sediment properties during IODP expeditions at no extra cost.
DOE Office of Scientific and Technical Information (OSTI.GOV)
P.C. Weaver
2009-04-29
The primary objective of the independent verification was to determine if BJC performed the appropriate actions to meet the specified “hot spot” cleanup criteria of 500 picocuries per gram (pCi/g) uranium-238 (U-238) in surface soil. Specific tasks performed by the independent verification team (IVT) to satisfy this objective included: 1) performing radiological walkover surveys, and 2) collecting soil samples for independent analyses. The independent verification (IV) efforts were designed to evaluate radioactive contaminants (specifically U-238) in the exposed surfaces below one foot of the original site grade, given that the top one foot layer of soil on the site wasmore » removed in its entirety.« less
Radionuclide concentrations in honey bees from Area G at TA-54 during 1997. Progress report
DOE Office of Scientific and Technical Information (OSTI.GOV)
Haarmann, T.K.; Fresquez, P.R.
Honey bees were collected from two colonies located at Los Alamos National Laboratory`s Area G, Technical Area 54, and from one control (background) colony located near Jamez Springs, NM. Samples were analyzed for the following: cesium ({sup 137}Cs), americium ({sup 241}Am), plutonium ({sup 238}Pu and {sup 239,240}Pu), tritium ({sup 3}H), total uranium, and gross gamma activity. Area G sample results from both colonies were higher than the upper (95%) level background concentration for {sup 238}Pu and {sup 3}H.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Sahoo, Sarata K.; Enomoto, Hiroko; Tokonami, Shinji
2008-08-07
Lichen and Moss are widely used to assess the atmospheric pollution by heavy metals and radionuclides. In this paper, we report results of uranium and its isotope ratios using mass spectrometric measurements (followed by chemical separation procedure) for mosses, lichens and soil samples from a depleted uranium (DU) target site in western Balkan region. Samples were collected in 2003 from Han Pijesak (Republika Srpska in Bosnia and Hercegovina). Inductively coupled plasma mass spectrometry (ICP-MS) measurements show the presence of high concentration of uranium in some samples. Concentration of uranium in moss samples ranged from 5.2-755.43 Bq/Kg. We have determined {supmore » 235}U/{sup 238}U isotope ratio using thermal ionization mass spectrometry (TIMS) from the samples with high uranium content and the ratios are in the range of 0.002097-0.002380. TIMS measurement confirms presence of DU in some samples. However, we have not noticed any traces of DU in samples containing lesser amount of uranium or from any samples from the living environment of same area.« less
Modeling of point defects and rare gas incorporation in uranium mono-carbide
NASA Astrophysics Data System (ADS)
Chartier, A.; Van Brutzel, L.
2007-02-01
An embedded atom method (EAM) potential has been established for uranium mono-carbide. This EAM potential was fitted on structural properties of metallic uranium and uranium mono-carbide. The formation energies of point defects, as well as activation energies for self migration, have been evaluated in order to cross-check the suitability of the potential. Assuming that the carbon vacancies are the main defects in uranium mono-carbide compounds, the migration paths and energies are consistent with experimental data selected by Catlow[C.R.A. Catlow, J. Nucl. Mater. 60 (1976) 151]. The insertion and migration energies for He, Kr and Xe have also been evaluated with available inter-atomic potentials [H.H. Andersen, P. Sigmund, Nucl. Instr. and Meth. B 38 (1965) 238]. Results show that the most stable defect configuration for rare gases is within uranium vacancies. The migration energy of an interstitial Xe is 0.5 eV, in agreement with the experimental value of 0.5 eV [Hj. Matzke, Science of advanced LMFBR fuels, Solid State Physics, Chemistry and Technology of Carbides, Nitrides and Carbonitrides of Uranium and Plutonium, North-Holland, 1986].
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.
NASA Astrophysics Data System (ADS)
Pereira, Wagner de S.; Kelecom, Alphonse; Py Júnior, Delcy de Azevedo
2008-08-01
The uranium mining at Caetité (Uranium Concentrate Unit—URA) is in its operational phase. Aiming to estimate the radiological environmental impact of the URA, a monitoring program is underway. In order to preserve the biota of the deleterious effects from radiation and to act in a pro-active way as expected from a licensing body, the present work aims to use an environmental protection methodology based on the calculation of absorbed dose rate in biota. Thus, selected target organism was the Tilapia fish (Tilapia nilotica, Linnaeus, 1758) and the radionuclides were: uranium (U-238), thorium (Th-232), radium (Ra-226 and Ra-228) and lead (Pb-210). As, in Brazil there are no radiation exposure limits adopted for biota the value proposed by the Department of Energy (DOE) of the United States of 3.5×103 μGy y-1 has been used. The derived absorbed dose rate calculated for Tilapia was 2.51×100 μGy y-1, that is less than 0.1% of the dose limit established by DOE. The critical radionuclide was Ra-226, with 56% of the absorbed dose rate, followed by U-238 with 34% and Th-232 with 9%. This value of 0.1% of the limit allows to state that, in the operational conditions analyzed, natural radionuclides do not represent a radiological problem to biota.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Pereira, Wagner de S; Universidade Federal Fluminense, Programa de Pos-graduacao em Biologia Marinha; Kelecom, Alphonse
2008-08-07
The uranium mining at Caetite (Uranium Concentrate Unit--URA) is in its operational phase. Aiming to estimate the radiological environmental impact of the URA, a monitoring program is underway. In order to preserve the biota of the deleterious effects from radiation and to act in a pro-active way as expected from a licensing body, the present work aims to use an environmental protection methodology based on the calculation of absorbed dose rate in biota. Thus, selected target organism was the Tilapia fish (Tilapia nilotica, Linnaeus, 1758) and the radionuclides were: uranium (U-238), thorium (Th-232), radium (Ra-226 and Ra-228) and lead (Pb-210).more » As, in Brazil there are no radiation exposure limits adopted for biota the value proposed by the Department of Energy (DOE) of the United States of 3.5x10{sup 3} {mu}Gy y{sup -1} has been used. The derived absorbed dose rate calculated for Tilapia was 2.51x10{sup 0} {mu}Gy y{sup -1}, that is less than 0.1% of the dose limit established by DOE. The critical radionuclide was Ra-226, with 56% of the absorbed dose rate, followed by U-238 with 34% and Th-232 with 9%. This value of 0.1% of the limit allows to state that, in the operational conditions analyzed, natural radionuclides do not represent a radiological problem to biota.« less
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.
Annamalai, Sathesh Kumar; Arunachalam, Kantha Deivi; Selvaraj, Rajaram
2017-06-01
Ten sampling locations in Nagarjuna Sagar Dam have been selected to assess the suitability of the reservoir water for human consumption. The sediment, water, and fish samples were collected and analyzed for radionuclide ( 238 U, 232 Th, 210 Po, 226 Ra, 210 Pb) and physicochemical parameters like pH, TOC, total hardness, alkalinity, DO, cation exchange capacity, and particle size. The spatial variations among the radionuclides ( 238 U, 232 Th, 210 Po, 226 Ra, 210 Pb) in water and bottom sediments of Nagarjuna Sagar Dam were determined. The uranium concentration in the sediment and water was in BDL (<0.5 ppb). The maximum permissible limits in water samples of the analyzed radionuclides are 238 U-10 Bq/l, 210 Po-0.1 Bq/l, 226 Ra-1 Bq/l, and 210 Pb-0.1 Bq/l. The radionuclides in our water samples were approximately 50 times far below the recommended limit. The ingestion of water and fish would not pose any significant radiological impact on health or cancer risk to the public, implicating that the fishes from Nagarjuna Sagar Dam reservoir are safe for human consumption except the fisherman community.
NASA Astrophysics Data System (ADS)
Kayzar, T. M.; Nelson, B. K.; Bachmann, O.; Portnyagin, M.; Ponomareva, V.
2010-12-01
Disequilibria in the short-lived uranium-series isotopic system can provide timescales of magma production, modification and transport in all tectonic settings. In volcanic arcs, the field has converged on the concept that (238U/230Th) and (226Ra/230Th) activities greater than one are a result of fluid fluxing from the slab to mantle wedge, and that the preservation of (226Ra/230Th) disequilibria requires rapid transport of melts from the mantle wedge to the surface (226Ra returns to equilibrium with 230Th in ~8000 years). The need for rapid transport coupled with the incompatibility of U-series elements suggest that U-series fractionation is not measurably affected by crustal processes. However, some well-studied arc systems, including the very productive Central Kamchatka Depression (CKD) of the Kamchatkan volcanic arc, show U-series data that are in conflict with this commonly accepted model. Our study focuses on two neighboring volcanic systems, Bezymianny and Klyuchevskoy volcanoes in the CKD. Separated by ~10km, these two systems are thought to share the same mantle source. Klyuchevskoy has primitive compositions (51-56 wt%) while Bezymianny erupts more differentiated andesites (57-63 wt% SiO2); therefore, by examining the U-series signals in these two systems it is possible to decouple a primary signal from one having undergone crustal processing. We record whole rock (238U/230Th) values for Bezymianny ranging from 0.94 to 0.96 in modern eruptive products, while (226Ra/230Th) are >1. We also observe a similar signal in older (212-6791BP) tephra deposits from Klyuchevskoy, measuring (238U/230Th) of 0.92-0.99 (unpublished data, collaborative research with the KALMAR project). (238U/230Th) <1 in arcs have mostly been reported from areas of thick continental crust (Andes; Sigmarsson et al. 1998, Garrison et al. 2006, Jicha et al. 2007) or from an arc where phases such as garnet and/or Al-rich clinopyroxene can retain a high U/Th in the crystalline residue (Jicha et al. 2009). Bezymianny and Klyuchevskoy have low Sr/Y (15.5-19.9), which precludes a significant influence of garnet in generating the observed Th-excess in the CKD. We investigate the possibility of shallow crustal processes such as fractional crystallization, and/or assimilation of local bulk rock or partial melts to fractionate U, Th, and Ra from one another. In particular, we focus on minor mineral phases, such as apatite and magnetite, which are present during early stages of differentiation (andesites) and may fractionate U from Th. We measure U and Th content in these phases in-situ by LA-ICP-MS to obtain average mineral-melt partitioning for each sample with U-series data. Using such average partition coefficients allows us to take into account variations in parameters such as temperature, pressure, and oxygen fugacity that may vary from sample to sample. This mineral trace element data is supported by bulk rock geochemistry and Pb isotope data to evaluate the effects of crustal processing on the U-series system during magma transport and storage.
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.
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.
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
NASA Astrophysics Data System (ADS)
Farmer, John G.; MacKenzie, Angus B.; Graham, Margaret C.; Macgregor, Kenneth; Kirika, Alexander
2015-05-01
The use of stable Pb isotope analyses in conjunction with recent (210Pb and anthropogenic radionuclide) chronologies has become a well-established method for evaluating historical trends in depositional fluxes and sources of atmospherically deposited Pb using archival records in lake sediment or peat cores. Such studies rely upon (i) simple radioactive disequilibrium between unsupported 210Pb and longer-lived members of the 238U decay series and (ii) well-defined values for the isotopic composition of contaminant Pb and indigenous Pb in the study area. However, areas of high natural radioactivity can present challenging environments for such studies, with potential complications arising from more complex disequilibria in the 238U decay series and the occurrence, at local or regional level, of anomalous, ill-defined stable isotope ratios due to the presence of elevated levels of radiogenic Pb. Results are presented here for a study of a sediment core from a freshwater lake, Loch Einich, in the high natural radioactivity area of the Cairngorm Mountains of Scotland. 238U decay series disequilibria revealed recent diagenetic re-deposition of both U and 226Ra, the latter resulting in a requirement to use a modified calculation to derive a 210Pb chronology for the core. Confidence in the chronology was provided by good agreement with the independent 241Am chronology, but the 137Cs distribution was affected by significant post-depositional mobility in the organic-rich sediment. The systematics of variations in 230Th, 232Th and stable Pb isotope ratio distributions were used to establish the indigenous Pb characteristics of the sediment. The relatively high radiogenic content of the indigenous Pb resulted in complications in source apportionment, in particular during the 20th century, with multiple natural and anthropogenic sources precluding the use of a simple binary mixing model. Consequently, 206Pb/207Pb ratios in Scottish moss samples from an archive collection were used to provide the input term for atmospheric deposition in order to establish historical trends in indigenous and anthropogenic Pb fluxes. A test of the accuracy of the derived Pb fluxes was provided by analysis of a core from a nearby blanket peat deposit, Great Moss. Independent atmospheric and basal inputs gave a complex distribution of 210Pb in the peat, but this did not affect calculation of a 210Pb chronology. Once again, the 210Pb chronology was supported by the 241Am distribution. Temporal trends in anthropogenic Pb deposition derived for the Loch Einich sediment core were in generally good agreement with those for the Great Moss peat core, other peat cores and some other lake sediment cores from northern Scotland, providing confidence in the use of the archive moss data to characterise atmospheric deposition. However, sustained input of Pb to Loch Einich sediment at relatively high levels in the late 20th century, after the regional decline in atmospheric Pb deposition, suggested that catchment-derived Pb is now a significant component of the depositional flux for Loch Einich.
Verçosa, Cícero Jorge; Moraes Filho, Aroldo Vieira de; Castro, Ícaro Fillipe de Araújo; Santos, Robson Gomes Dos; Cunha, Kenya Silva; Silva, Daniela de Melo E; Garcia, Ana Cristina Lauer; Navoni, Julio Alejandro; Amaral, Viviane Souza do; Rohde, Claudia
2017-07-01
Natural radiation of geological origin is a common phenomenon in Brazil, a country where radioactive agents such as uranium may be often found. As an unstable atom, uranium undergoes radioactive decay with the generation of a series of decay by-products, including radon, which may be highly genotoxic and trigger several pathological processes, among which cancer. Because it is a gas, radon may move freely between cracks and gaps in the ground, seeping upwards into the buildings and in the environment. In this study, two Drosophila melanogaster Meigen (Diptera, Drosophilidae) strains called Oregon-R and Wild (collected in a non-radioactive environment) were exposed to atmospheric radiation in the Lajes Pintadas city, in the semiarid zone of northeastern Brazil. After six days of environmental exposure, the organisms presented genetic damage significantly higher than that of the negative control group. The genotoxic effects observed reinforce the findings of other studies carried out in the same region, which warn about the environmental risks related to natural radioactivity occurrence. The results also validate the use of the Comet assay in hemocytes of D. melanogaster as a sensitive test to detect genotoxicity caused by natural radiation, and the use of a recently collected D. melanogaster strain in the environmental of radon. Copyright © 2017. Published by Elsevier Inc.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Isselhardt, B. H.; Prussin, S. G.; Savina, M. R.
2016-01-01
Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process between uranium atoms and potential isobars without the aid of chemical purification and separation. The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of the U-235/U-238 ratio to decrease laser-induced isotopic fractionation. In application, isotope standards are used to identify and correct bias in measured isotope ratios, but understanding laser-induced bias from first-principles can improve the precision and accuracy of experimental measurements. A rate equationmore » model for predicting the relative ionization probability has been developed to study the effect of variations in laser parameters on the measured isotope ratio. The model uses atomic data and empirical descriptions of laser performance to estimate the laser-induced bias expected in experimental measurements of the U-235/U-238 ratio. Empirical corrections are also included to account for ionization processes that are difficult to calculate from first principles with the available atomic data. Development of this model has highlighted several important considerations for properly interpreting experimental results.« less
Isselhardt, B. H.; Prussin, S. G.; Savina, M. R.; ...
2015-12-07
Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process between uranium atoms and potential isobars without the aid of chemical purification and separation. The use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of the 235U/238U ratio to decrease laser-induced isotopic fractionation. In application, isotope standards are used to identify and correct bias in measured isotope ratios, but understanding laser-induced bias from first-principles can improve the precision and accuracy of experimental measurements. A rate equationmore » model for predicting the relative ionization probability has been developed to study the effect of variations in laser parameters on the measured isotope ratio. The model uses atomic data and empirical descriptions of laser performance to estimate the laser-induced bias expected in experimental measurements of the 235U/ 238U ratio. Empirical corrections are also included to account for ionization processes that are difficult to calculate from first principles with the available atomic data. As a result, development of this model has highlighted several important considerations for properly interpreting experimental results.« less
Processing of irradiated, enriched uranium fuels at the Savannah River Plant
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hyder, M L; Perkins, W C; Thompson, M C
Uranium fuels containing /sup 235/U at enrichments from 1.1% to 94% are processed and recovered, along with neptunium and plutonium byproducts. The fuels to be processed are dissolved in nitric acid. Aluminum-clad fuels are disssolved using a mercury catalyst to give a solution rich in aluminum. Fuels clad in more resistant materials are dissolved in an electrolytic dissolver. The resulting solutions are subjected to head-end treatment, including clarification and adjustment of acid and uranium concentration before being fed to solvent extraction. Uranium, neptunium, and plutonium are separated from fission products and from one another by multistage countercurrent solvent extraction withmore » dilute tri-n-butyl phosphate in kerosene. Nitric acid is used as the salting agent in addition to aluminum or other metal nitrates present in the feed solution. Nuclear safety is maintained through conservative process design and the use of monitoring devices as secondary controls. The enriched uranium is recovered as a dilute solution and shipped off-site for further processing. Neptunium is concentrated and sent to HB-Line for recovery from solution. The relatively small quantities of plutonium present are normally discarded in aqueous waste, unless the content of /sup 238/Pu is high enough to make its recovery desirable. Most of the /sup 238/Pu can be recovered by batch extraction of the waste solution, purified by counter-current solvent extraction, and converted to oxide in HB-Line. By modifying the flowsheet, /sup 239/Pu can be recovered from low-enriched uranium in the extraction cycle; neptunium is then not recovered. The solvent is subjected to an alkaline wash before reuse to remove degraded solvent and fission products. The aqueous waste is concentrated and partially deacidified by evaporation before being neutralized and sent to the waste tanks; nitric acid from the overheads is recovered for reuse.« less
Americium As A Potential Power Source For Space Missions
NASA Astrophysics Data System (ADS)
Cordingley, Leon; Rice, Tom; Sarsfield, Mark J.; Stephenson, Keith; Tinsley, Tim
2011-10-01
Electrical power sources used in outer planet missions are a key enabling technology for data acquisition and communications. Power sources generate electricity from the thermal energy from alpha decay of the radioisotope 238Pu via thermoelectric conversion. Production of 238Pu requires specialist facilities including a nuclear reactor and reprocessing plants that are expensive to build and operate, so naturally, a more economical alternative is attractive to the industry. Within Europe 241Am is a feasible alternative to 238Pu that can provide a heat source for radioisotope thermoelectric generators (RTGs) and radioisotope heating units (RHUs). Whilst there are implications associated with the differences between 238Pu and 241Am, these technological challenges are surmountable.
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
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.
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
Lenka, Pradyumna; Sahoo, S K; Mohapatra, S; Patra, A C; Dubey, J S; Vidyasagar, D; Tripathi, R M; Puranik, V D
2013-03-01
A natural high background radiation area is located in Chhatrapur, Odisha in the eastern part of India. The inhabitants of this area are exposed to external radiation levels higher than the global average background values, due to the presence of uranium, thorium and its decay products in the monazite sands bearing placer deposits in its beaches. The concentrations of (232)Th, (238)U, (226)Ra, (40)K and (137)Cs were determined in cereals (rice and wheat), pulses and drinking water consumed by the population residing around this region and the corresponding annual ingestion dose was calculated. The annual ingestion doses from cereals, pulses and drinking water varied in the range of 109.4-936.8, 10.2-307.5 and 0.5-2.8 µSv y(-1), respectively. The estimated total annual average effective dose due to the ingestion of these radionuclides in cereals, pulses and drinking water was 530 µSv y(-1). The ingestion dose from cereals was the highest mainly due to a high consumption rate. The highest contribution of dose was found to be from (226)Ra for cereals and drinking water and (40)K was the major dose contributor from the intake of pulses. The contribution of man-made radionuclide (137)Cs to the total dose was found to be minimum. (226)Ra was found to be the largest contributor to ingestion dose from all sources.
Uranium: A Dentist's perspective
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
Distribution of uranium and some selected trace metals in human scalp hair from Balkans.
Zunic, Z S; Tokonami, S; Mishra, S; Arae, H; Kritsananuwat, R; Sahoo, S K
2012-11-01
The possible consequences of the use of depleted uranium (DU) used in Balkan conflicts in 1995 and 1999 for the people and the environment of this reason need attention. The heavy metal content in human hair may serve as a good indicator of dietary, environmental and occupational exposures to the metal compounds. The present work summarises the distribution of uranium and some selected trace metals such as Mn, Ni, Cu, Zn, Sr, Cd and Cs in the scalp hair of inhabitants from Balkans exposed to DU directly and indirectly, i.e. Han Pijesak, Bratoselce and Gornja Stubla areas. Except U and Cs, all other metals were compared with the worldwide reported values of occupationally unexposed persons. Uranium concentrations show a wide variation ranging from 0.9 ± 0.05 to 449 ± 12 µg kg(-1). Although hair samples were collected from Balkan conflict zones, uranium isotopic measurement ((235)U/(238)U) shows a natural origin rather than DU.
Caves, mines and subterranean spaces: hazard and risk from exposure to radon.
NASA Astrophysics Data System (ADS)
Crockett, R. G. M.; Gillmore, G. K.
2009-04-01
Radon is a naturally occurring radioactive gas. It is colourless, odourless and chemically inert. The most hazardous isotope is 222Rn. Radon is formed in the natural environment by the radioactive decay of the element uranium (238U) and is a daughter product of daughter product of radium (226Ra). Uranium and radium are found, in differing degrees, in a wide range of rocks, soils (and building materials that are made from these). Radon concentrations in caves, e.g. limestone caves such as the Great Cave of Niah, Borneo, and caves in the Mendips and Peak District in the UK, has been documented and reveal that both (prehistoric) cave-dwellers and other users such as archaeologists are at risk from exposure to radon a naturally occurring radioactive gas. In general, but dependent on cave geometry and ventilation, radon concentration increases with increasing distance from the entrance, implying that the hazard also increases with distance from the entrance. With regard to mines and mining operations, as well as modern extraction of uranium and radium ores, both ores commonly occur alongside other metallic ores, e.g. silver at Schneeberg and Joachimsthal, and tin in Cornwall, and in some instances, waste from earlier metalliferious mining activity has itself been ‘mined' for uranium and/or radium ores. It is not solely the miners and other subterranean workers which are at risk, other workers and local inhabitants are also at risk. Also, that risk is not eliminated by protection against dust/airborne particulates: the risk from inhalation of radon is only reduced by reducing the inhalation of radon, i.e. use of breathing apparatus. Amongst the general population, radon is the second most significant cause of lung cancer behind tobacco smoking. Estimates vary but 6-9% of lung-cancers are attributable to radon and approximately 2% all cancer deaths are attributable to radon. These proportions will increase in higher-radon environments such as caves, mines and mining areas (via spoil heaps, settlement lagoons etc. containing uranium and radium). We here present an overview of the potential hazard presented by radon in subterranean spaces and by metalliferous mining activities. We also present some speculation as to evidence of (pre-) historic exposure to radon which might potentially exist in archaeological remains and oral traditions. Keywords: radon; caves; metalliferous mining; cave-dwellers; archaeologists.
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.
Vandenhove, H; Van Hees, M; Wouters, K; Wannijn, J
2007-01-01
Present study aims to quantify the influence of soil parameters on soil solution uranium concentration for (238)U spiked soils. Eighteen soils collected under pasture were selected such that they covered a wide range for those parameters hypothesised as being potentially important in determining U sorption. Maximum soil solution uranium concentrations were observed at alkaline pH, high inorganic carbon content and low cation exchange capacity, organic matter content, clay content, amorphous Fe and phosphate levels. Except for the significant correlation between the solid-liquid distribution coefficients (K(d), L kg(-1)) and the organic matter content (R(2)=0.70) and amorphous Fe content (R(2)=0.63), there was no single soil parameter significantly explaining the soil solution uranium concentration (which varied 100-fold). Above pH=6, log(K(d)) was linearly related with pH [log(K(d))=-1.18 pH+10.8, R(2)=0.65]. Multiple linear regression analysis did result in improved predictions of the soil solution uranium concentration but the model was complex.
β-decay Rates for Exotic Nuclei and r-process Nucleosynthesis up to Thorium and Uranium
NASA Astrophysics Data System (ADS)
Suzuki, Toshio; Shibagaki, Shota; Yoshida, Takashi; Kajino, Toshitaka; Otsuka, Takaharu
2018-06-01
Beta-decay rates for exotic nuclei with neutron magic number of N = 126 relevant to r-process nucleosynthesis are studied up to Z = 78 by shell-model calculations. The half-lives for the waiting-point nuclei obtained, which are short compared to a standard finite-range-droplet model, are used to study r-process nucleosynthesis in core-collapse supernova (CCSN) explosions and binary neutron star mergers. The element abundances are obtained up to the third peak as well as beyond the peak region up to thorium and uranium. The position of the third peak is found to be shifted toward a higher mass region in both CCSN explosions and neutron star mergers. We find that thorium and uranium elements are produced more with the shorter shell-model half-lives and their abundances come close to the observed values in CCSN explosions. In the case of binary neutron star mergers, thorium and uranium are produced consistently with the observed values independent of the half-lives.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bernard, David; Leconte, Pierre; Destouches, Christophe
2015-07-01
Two recent papers justified a new experimental program to give a new basis for the validation of {sup 238}U nuclear data, namely neutron induced inelastic scattering and transport codes at neutron fission energies. The general idea is to perform a neutron transmission experiment through natural uranium material. As shown by Hans Bethe, neutron transmissions measured by dosimetric responses are linked to inelastic cross sections. This paper describes the principle and the results of such an experience called EXCALIBUR performed recently (January and October 2014) at the CALIBAN reactor facility. (authors)
Hybrid interferometric/dispersive atomic spectroscopy of laser-induced uranium plasma
Morgan, Phyllis K.; Scott, Jill R.; Jovanovic, Igor
2015-12-19
An established optical emission spectroscopy technique, laser-induced breakdown spectroscopy (LIBS), holds promise for detection and rapid analysis of elements relevant for nuclear safeguards, nonproliferation, and nuclear power, including the measurement of isotope ratios. One such important application of LIBS is the measurement of uranium enrichment ( 235U/ 238U), which requires high spectral resolution (e.g., 25 pm for the 424.4 nm U II line). High-resolution dispersive spectrometers necessary for such measurements are typically bulky and expensive. We demonstrate the use of an alternative measurement approach, which is based on an inexpensive and compact Fabry–Perot etalon integrated with a low to moderatemore » resolution Czerny–Turner spectrometer, to achieve the resolution needed for isotope selectivity of LIBS of uranium in ambient air. Furthermore, spectral line widths of ~ 10 pm have been measured at a center wavelength 424.437 nm, clearly discriminating the natural from the highly enriched uranium.« less
Uranium plasma emission at gas-core reaction conditions
NASA Technical Reports Server (NTRS)
Williams, M. D.; Jalufka, N. W.; Hohl, F.; Lee, J. H.
1976-01-01
The results of uranium plasma emission produced by two methods are reported. For the first method a ruby laser was focused on the surface of a pure U-238 sample to create a plasma plume with a peak plasma density of about 10 to the 20th power/cu cm and a temperature of about 38,600 K. The absolute intensity of the emitted radiation, covering the range from 300 to 7000 A was measured. For the second method, the uranium plasma was produced in a 20 kilovolt, 25 kilojoule plasma-focus device. The 2.5 MeV neutrons from the D-D reaction in the plasma focus are moderated by polyethylene and induce fissions in the U-235. Spectra of both uranium plasmas were obtained over the range from 30 to 9000 A. Because of the low fission yield the energy input due to fissions is very small compared to the total energy in the plasma.
Uranium plasma radiates in the UV spectrum
NASA Technical Reports Server (NTRS)
Williams, M. D.
1973-01-01
Description of an experiment designed to produce and spectroscopically analyze a simulated gas core reactor plasma in the spectral range from 300 to 1300 A. The plasma was produced by focusing the radiation of a Q-spoiled ruby laser onto the flat surface of a pure U-238 specimen.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Robison, W L; Noshkin, V E; Hamilton, T F
2001-05-01
Different stable elements, and some natural and man-made radionuclides, were used as tracers or associated in other ways with nuclear devices that were detonated at Bikini and Enewetak Atolls as part of the U.S. nuclear testing program from 1946 through 1958. The question has been raised whether any of these materials dispersed by the explosions could be of sufficient concentration in either the marine environment or on the coral islands to be of a health concern to people living, or planning to live, on the atolls. This report addresses that concern. An inventory of the materials involved during the testmore » period was prepared and provided to us by the Office of Defense Programs (DP) of the United States Department of Energy (DOE). The materials that the DOE and the Republic of the Marshall Islands (RMI) ask to be evaluated are--sulfur, arsenic, yttrium, tantalum, gold, rhodium, indium, tungsten, thallium, thorium-230,232 ({sup 230,232}Th), uranium-233,238 ({sup 233,238}U), polonium-210 ({sup 210}Po), curium-232 ({sup 232}Cu), and americium-241 ({sup 241}Am). The stable elements were used primarily as tracers for determining neutron energy and flux, and for other diagnostic purposes in the larger yield, multistage devices. It is reasonable to assume that these materials would be distributed in a similar manner as the fission products subsequent to detonation. A large inventory of fission product and uranium data was available for assessment. Detailed calculations show only a very small fraction of the fission products produced during the entire test series remain at the test site atolls. Consequently, based on the information provided, we conclude that the concentration of these materials in the atoll environment pose no adverse health effects to humans.« less
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
Natural radionuclides in trees grown on a uranium mill tailings waste pile.
Strok, Marko; Smodiš, Borut; Eler, Klemen
2011-06-01
The purpose of the study was to investigate natural radionuclide uptake and allocation by trees. Samples from six Scots pines (P. sylvestris), six Norway spruces (Picea abies) and one sycamore maple (Acer pseudoplatanus) tree, growing on the Boršt uranium mill tailings waste pile in Slovenia were collected. (238)U, (230)Th, (226)Ra and (210)Pb activity concentrations in wood, shoots and 1-year-old needles or leaves were determined. Particular radionuclides were separated from the samples by appropriate radiochemical procedures and their activity concentrations measured with an alpha spectrometry system. In addition, concentration ratios for different plant parts were calculated. Results showed that for all radionuclides, the highest activity concentrations were found in foliage, followed by shoots and wood. The activity concentrations in trees were from 0.01 to 5.4 Bq kg(-1) for (238)U, 0.03-11.3 Bq kg(-1) for (230)Th, 2.7-2,728 Bq kg(-1) for (226)Ra and 5.1-321 Bq kg(-1) for (210)Pb. All activity concentrations were calculated on dry weight basis. The calculated concentration ratios were from 1.05E-5 to 5.39E-3 for (238)U, 7.65E-6-2.88E-3 for (230)Th, 3.10E-4-3.16E-1 for (226)Ra and 6.70E-4-4.22E-2 for (210)Pb.
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.
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.
Measurement of intrinsic radioactive backgrounds from the 137Cs and U/Th chains in CsI(Tl) crystals
NASA Astrophysics Data System (ADS)
Liu, Shu-Kui; Yue, Qian; Lin, Shin-Ted; Li, Yuan-Jing; Tang, Chang-Jian; Wong Tsz-King, Henry; Xing, Hao-Yang; Yang, Chao-Wen; Zhao, Wei; Zhu, Jing-Jun
2015-04-01
The inorganic CsI(Tl) crystal scintillator is a candidate anti-compton detector for the China Dark matter Experiment. Studying the intrinsic radiopurity of the CsI(Tl) crystal is an issue of major importance. The timing, energy and spatial correlations, as well as the capability of pulse shape discrimination provide powerful methods for the measurement of intrinsic radiopurities. The experimental design, detector performance and event-selection algorithms are described. A total of 359×3 kg-days data from three prototypes of CsI(Tl) crystals were taken at China Jinping Underground Laboratory (CJPL), which offers a good shielding environment. The contamination levels of internal isotopes from 137Cs, 232Th and 238U series, as well as the upper bounds of 235U series are reported. Identification of the whole α peaks from U/Th decay chains and derivation of those corresponding quenching factors are achieved. Supported by National Natural Science Foundation of China (11275107, 11175099)
Measurement of Geo-neutrinos with KamLAND
DOE Office of Scientific and Technical Information (OSTI.GOV)
Yamada, Satoru
2011-11-23
Radioactive isotopes inside the Earth produce geo-neutrinos through beta decays. Geo-neutrinos could be direct probes to investigate the interior of the Earth as a supplement to the current geophysical survey that mainly relies on an indirect seismic approach. After the Kamioka liquid scintillator antineutrino detector (KamLAND) reported the first indication of geo-neutrinos in 2005, we have accumulated data for a total of 2,135 days of live-time and achieved a lower background level by purifying liquid scintillator. The number of obtained geo-neutrino events is 106{sub -28}{sup +29} corresponding to an electron antineutrino flux of 4.3{sub -1.1}{sup +1.2}x10{sup 6} cm{sup -2} s{supmore » -1} from {sup 238}U and {sup 232}Th series at the Earth's surface. The null hypothesis for the existence of geo-neutrinos is excluded at the 99.997% confidence level. We combined this precise result with that of the Borexino experiment to obtain 20.0{sub -8.6}{sup +8.8} TW as a contribution of {sup 238}U and {sup 232}Th to the Earth heat flow.« less
General-Purpose Heat Source Safety Verification Test Program: Edge-on flyer plate tests
NASA Astrophysics Data System (ADS)
George, T. G.
1987-03-01
The radioisotope thermoelectric generator (RTG) that will supply power for the Galileo and Ulysses space missions contains 18 General-Purpose Heat Source (GPHS) modules. The GPHS modules provide power by transmitting the heat of Pu-238 alpha-decay to an array of thermoelectric elements. Each module contains four Pu-238O2-fueled clads and generates 250 W(t). Because the possibility of a launch vehicle explosion always exists, and because such an explosion could generate a field of high-energy fragments, the fueled clads within each GPHS module must survive fragment impact. The edge-on flyer plate tests were included in the Safety Verification Test series to provide information on the module/clad response to the impact of high-energy plate fragments. The test results indicate that the edge-on impact of a 3.2-mm-thick, aluminum-alloy (2219-T87) plate traveling at 915 m/s causes the complete release of fuel from capsules contained within a bare GPHS module, and that the threshold velocity sufficient to cause the breach of a bare, simulant-fueled clad impacted by a 3.5-mm-thick, aluminum-alloy (5052-TO) plate is approximately 140 m/s.
Age of the moon: An isotopic study of uranium-thorium-lead systematics of lunar samples
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.
Radiation protection and radioactive scales in oil and gas production.
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.
Health investigations of depleted-uranium clean-up workers.
Milacic, Snezana
2008-01-01
The soil contaminated by depleted uranium (238U) ammunition during the NATO bombing of Serbia and Montenegro was cleaned-up for four months in 2002. A team of 11 clean-up workers (expert members) were medically examined three times: before decontamination as a preliminary medical check-up, immediately after decontamination, and four years after cleaning up contaminated ground. This short report presents investigations and health risk assessments of clean-up workers in radioactive decontamination operations and an assessment of the environmental health perspectives for citizens living in surrounding areas. The method of initial health disorders was used, analyzing the most sensitive biological materials, such as blood cells or chromosome damage, DNA strand breaks, radio-toxicological examination of urine. The total number of blood cells did not change, but variations of the relative number (percentage) of cells in the leukocyte formula were observed. The total number of DNA alterations was higher immediately after decontamination than before decontamination. Four years after decontamination the number of DNA alterations had decreased. However, the number of damaged cells (lymphocytes containing chromosome lesions) was higher in both medical examinations, immediately after and four years after decontamination. Disease or tumours due to 238U did not develop in the group of depleted uranium clean-up workers during the investigation period of four years. Further monitoring of haematological and chromosomal effects and the health condition of workers is necessary.
Direct uranium isotope ratio analysis of single micrometer-sized glass particles
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
Direct uranium isotope ratio analysis of single micrometer-sized glass particles.
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.
Meinrath, A; Schneider, P; Meinrath, G
2003-01-01
The Erzgebirge ('Ore Mountains') area in the eastern part of Germany was a major source of uranium for Soviet nuclear programs between 1945 and 1989. During this time, the former German Democratic Republic became the third largest uranium producer in the world. The high abundance of uranium in the geological formations of the Erzgebirge are mirrored in the discovery of uranium by M. Klaproth close to Freiberg City in 1789 and the description of the so-called 'Schneeberg' disease, lung cancer caused in miners by the accumulation of the uranium decay product, radon, in the subsurfaces of shafts. Since 1991, remediation and mitigation of uranium at production facilities, rock piles and mill tailings has taken place. In parallel, efforts were initiated to assess the likely adverse effects of uranium mining to humans. The costs of these activities amount to about 6.5 10(9) Euro. A comparison with concentrations of depleted uranium at certain sites is given.
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.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Duke, Dana Lynn
2015-11-12
This Ph.D. dissertation describes a measurement of the change in mass distributions and average total kinetic energy (TKE) release with increasing incident neutron energy for fission of 235U and 238U. Although fission was discovered over seventy-five years ago, open questions remain about the physics of the fission process. The energy of the incident neutron, En, changes the division of energy release in the resulting fission fragments, however, the details of energy partitioning remain ambiguous because the nucleus is a many-body quantum system. Creating a full theoretical model is difficult and experimental data to validate existing models are lacking. Additional fissionmore » measurements will lead to higher-quality models of the fission process, therefore improving applications such as the development of next-generation nuclear reactors and defense. This work also paves the way for precision experiments such as the Time Projection Chamber (TPC) for fission cross section measurements and the Spectrometer for Ion Determination in Fission (SPIDER) for precision mass yields.« less
Muhs, D.R.; Kennedy, G.L.
1985-01-01
Fossil sea urchins (Strongylocentrotus) from Pleistocene marine terraces on the southern California Channel Islands have been dated by the uranium-series method in order to test the suitability of echinoids for dating marine terraces. Results indicate that urchin plates and spines do not behave as closed systems with respect to both uranium and thorium. Calculated ages based on these data do not agree with uranium-series ages (120,000 and 127,000 yrs) obtained previously from corals from the same localities. Thus, fossil sea urchins (Strongylocentrotus) are not considered suitable for uraniumseries dating of Pleistocene marine terrace deposits. ?? 1985.
(234)U/(238)U signatures associated with uranium ore bodies: part 2 Manyingee.
Lowson, Richard T; McIntyre, Mark G
2013-04-01
The Manyingee ore body is a roll-front U ore body located at depth in the Cretaceous sandstone sediments of a Proterozoic palaeo valley. It is located in a confined aquifer. The aquifer is recharged 4 km upstream by the Ashburton River. Groundwater samples were collected at and up to 4.7 km downstream of the ore body. The ground water (234)U/(238)U activity ratios (AR) were elevated to 1.86 in the vicinity of the ore body and then declined to 1.06 over the 4.7 km transect. The elevated (234)U/(238)U ARs are attributed to selective leaching of (234)U sites by oxidising waters, with α recoil as a necessary precursor to produce activated (234)U sites. Direct ejection into another phase following α recoil is considered to be a minor contributor to (234)U -(238)U disequilibrium in this environment. The profile is considered to be typical of the (234)U/(238)U AR profile at and down gradient of the redox front of a U ore body. Crown Copyright © 2012. Published by Elsevier Ltd. All rights reserved.
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.
NASA Astrophysics Data System (ADS)
Willingham, David; Naes, Benjamin E.; Tarolli, Jay G.; Schemer-Kohrn, Alan; Rhodes, Mark; Dahl, Michael; Guzman, Anthony; Burkes, Douglas E.
2018-01-01
Uranium-molybdenum (U-Mo) monolithic fuels represent one option for converting civilian research and test reactors operating with high enriched uranium (HEU) to low enriched uranium (LEU), effectively reducing the threat of nuclear proliferation world-wide. However, processes associated with fabrication of U-Mo monolithic fuels result in regions of elemental heterogeneity, observed as bands traversing the cross-section of representative samples. Isotopic variations (e.g., 235U and 238U) could also be introduced because of associated processing steps, particularly since HEU feedstock is melted with natural or depleted uranium diluent to produce LEU. This study demonstrates the utility of correlative analysis of Energy-Dispersive X-ray Spectroscopy (EDS) and Secondary Ion Mass Spectrometry (SIMS) with their image data streams using image fusion, resulting in a comprehensive microanalytical characterization toolbox. Elemental and isotopic measurements were made on a sample from the Advanced Test Reactor (ATR) Full-sized plate In-center flux trap Position (AFIP)-7 experiment and compared to previous optical and electron microscopy results. The image fusion results are characteristic of SIMS isotopic maps, but with the spatial resolution of EDS images and, therefore, can be used to increase the effective spatial resolution of the SIMS imaging results to better understand homogeneity or heterogeneity that persists because of processing selections. Visual inspection using the image fusion methodology indicated slight variations in the 235U/238U ratio and quantitative analysis using the image intensities across several FoVs revealed an average 235U atom percent value of 17.9 ± 2.4%, which was indicative of a non-uniform U isotopic distribution in the area sampled. Further development of this capability is useful for understanding the connections between the properties of LEU fuel alternatives and the ability to predict performance under irradiation.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ullmann, John L; Couture, A J; Keksis, A L
2010-01-01
A careful new measurement of the {sup 238}U(n,{gamma}) cross section from 10 eV to 100 keV has been made using the DANCE detector at LANSCE. DANCE is a 4{pi} calorimetric scintillator array consisting of 160 BaF{sub 2} crystals. Measurements were made on a 48 mg/cm{sup 2} depleted uranium target. The cross sections are in general good agreement with previous measurements. The gamma-ray emission spectra, as a function of gamma multiplicity, were also measured and compared to model calculations.
NASA Astrophysics Data System (ADS)
Schilk, A. J.; Abel, K. H.; Brown, D. P.; Thompson, R. C.; Knopf, M. A.; Hubbard, C. W.
1994-04-01
A novel scintillating-fiber sensor for detecting high-energy beta particles has been designed and built at the Pacific Northwest Laboratory to characterize U-238 and Sr-90 in surface soils. High-energy betas generate unique signals as they pass through multiple layers of scintillating fibers that make up the active region of the detector. Lower-energy beta particles, gamma rays, and cosmic-ray-generated particles comprise the majority of the background interferences. The resulting signals produced by these latter phenomena are effectively discriminated against due to the combination of the sensor's multilayer configuration and its interlayer coincidence/anticoincidence circuitry.
A Graphical Examination of Uranium and Plutonium Fissility
ERIC Educational Resources Information Center
Reed, B. Cameron
2008-01-01
The issue of why only particular isotopes of uranium and plutonium are suitable for use in nuclear weapons is analyzed with the aid of graphs and semiquantitative discussions of parameters such as excitation energies, fission barriers, reaction cross-sections, and the role of processes such as [alpha]-decay and spontaneous fission. The goal is to…
NASA Astrophysics Data System (ADS)
Larijani, C.; Jerome, S. M.; Lorusso, G.; Ivanov, P.; Russell, B.; Pearce, A. K.; Regan, P. H.
2017-11-01
The aim of the current work is to develop and validate a radiochemical separation scheme capable of separating both 236gNp and 236Pu from a uranium target of natural isotopic composition ( 1 g uranium) and 200 MBq of fission decay products. A target containing 1.2 g of UO2 was irradiated with a beam of 25 MeV protons with a typical beam current of 30 μA for 19 h in December 2013 at the University of Birmingham Cyclotron facility. Using literature values for the production cross-section for fusion of protons with uranium targets, we estimate that an upper limit of approximately 250 Bq of activity from the 236Np ground state was produced in this experiment. Using a radiochemical separation scheme, Np and Pu fractions were separated from the produced fission decay products, with analyses of the target-based final reaction products made using Inductively Couple Plasma Mass Spectrometry (ICP-MS) and high-resolution α particle and γ-ray spectrometry.
Uranium decay daughters from isolated mines: Accumulation and sources.
Cuvier, A; Panza, F; Pourcelot, L; Foissard, B; Cagnat, X; Prunier, J; van Beek, P; Souhaut, M; Le Roux, G
2015-11-01
This study combines in situ gamma spectrometry performed at different scales, in order to accurately locate the contamination pools, to identify the concerned radionuclides and to determine the distribution of the contaminants from soil to bearing phase scale. The potential mobility of several radionuclides is also evaluated using sequential extraction. Using this procedure, an accumulation area located downstream of a former French uranium mine and concentrating a significant fraction of radioactivity is highlighted. We report disequilibria in the U-decay chains, which are likely related to the processes implemented on the mining area. Coupling of mineralogical analyzes with sequential extraction allow us to highlight the presence of barium sulfate, which may be the carrier of the Ra-226 activities found in the residual phase (Ba(Ra)SO4). In contrast, uranium is essentially in the reducible fraction and potentially trapped in clay-iron coatings located on the surface of minerals. Copyright © 2015 Elsevier Ltd. All rights reserved.
Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits
NASA Astrophysics Data System (ADS)
Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly D.; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan; Borch, Thomas
2017-06-01
Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U(VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U(IV) generated through biologically mediated U(VI) reduction is the predominant U(IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (~58-89%) of U is bound as U(IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U(VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotope signatures, consistent with largely biotic reduction of U(VI) to U(IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U(IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.
Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits
Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly D.; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan; Borch, Thomas
2017-01-01
Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U(VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U(IV) generated through biologically mediated U(VI) reduction is the predominant U(IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (∼58-89%) of U is bound as U(IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U(VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotope signatures, consistent with largely biotic reduction of U(VI) to U(IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U(IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment. PMID:28569759
Biogenic non-crystalline U (IV) revealed as major component in uranium ore deposits
Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly D.; ...
2017-06-01
Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U (VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U (IV) generated through biologically mediated U (VI) reduction is the predominant U (IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (~58-89%) of U is bound as U (IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U (VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotopemore » signatures, consistent with largely biotic reduction of U (VI) to U (IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U (IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.« less
Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits.
Bhattacharyya, Amrita; Campbell, Kate M; Kelly, Shelly D; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan; Borch, Thomas
2017-06-01
Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U (VI) ) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U (IV) generated through biologically mediated U (VI) reduction is the predominant U (IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (∼58-89%) of U is bound as U (IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U (VI) represent only minor components. The uranium deposit exhibited mostly 238 U-enriched isotope signatures, consistent with largely biotic reduction of U (VI) to U (IV) . This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U (IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.
Biogenic non-crystalline U (IV) revealed as major component in uranium ore deposits
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly D.
Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U (VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U (IV) generated through biologically mediated U (VI) reduction is the predominant U (IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (~58-89%) of U is bound as U (IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U (VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotopemore » signatures, consistent with largely biotic reduction of U (VI) to U (IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U (IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.« less
Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits
Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan; Borch, Thomas
2017-01-01
Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U(VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U(IV) generated through biologically mediated U(VI) reduction is the predominant U(IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (∼58-89%) of U is bound as U(IV)to C-containing organic functional groups or inorganic carbonate, while uraninite and U(VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotope signatures, consistent with largely biotic reduction of U(VI) to U(IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U(IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.
Geochemical hosts of solubilized radionuclides in uranium mill tailings
Landa, E.R.; Bush, C.A.
1990-01-01
The solubilization and subsequent resorption of radionuclides by ore components or by reaction products during the milling of uranium ores may have both economic and environmental consequences. Particle-size redistribution of radium during milling has been demonstrated by previous investigators; however, the identification of sorbing components in the tailings has received little experimental attention. In this study, uranium-bearing sandstone ore was milled, on a laboratory scale, with sulfuric acid. At regular intervals, filtrate from this suspension was placed in contact with mixtures of quartz sand and various potential sorbents which occur as gangue in uranium ores; the potential sorbents included clay minerals, iron and aluminum oxides, feldspar, fluorspar, barite, jarosite, coal, and volcanic glass. After equilibration, the quartz sand-sorbent mixtures were separated from the filtrate and radioassayed by gamma-spectrometry to determine the quantities of 238U, 230Th, 226Ra, and 210Pb sorbed, and the radon emanation coefficients. Sorption of 238U was low in all cases, with maximal sorptions of 1-2% by the bentonite- and coal-bearing samples. 230Th sorption also was generally less than 1%; maximal sorption here was observed in the fluorspar-bearing sample and appears to be associated with the formation of gypsum during milling. 226Ra and 210 Pb generally showed higher sorption than the other nuclides - more than 60% of the 26Ra solubilized from the ore was sorbed on the barite-bearing sample. The mechanism (s) for this sorption by a wide variety of substrates is not yet understood. Radon emanation coefficients of the samples ranged from about 5 to 30%, with the coal-bearing samples clearly demonstrating an emanating power higher than any of the other materials. ?? 1990.
Applied technology for mine waste water decontamination in the uranium ores extraction from Romania
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bejenaru, C.; Filip, G.; Vacariu, V.T.
1996-12-31
The exploitation of uranium ores in Romania is carried out in underground mines. In all exploited uranium deposits, mine waste waters results and will still result after the closure of uranium ore extraction activity. The mine waters are radioactively contaminated with uranium and its decay products being a hazard both for underground waters as for the environment. This paper present the results of research work carried out by authors for uranium elimination from waste waters as the problems involved during the exploitation process of the existent equipment as its maintenance in good experimental conditions. The main waste water characteristics aremore » discussed: solids as suspension, uranium, radium, mineral salts, pH, etc. The moist suitable way to eliminate uranium from mine waste waters is the ion exchange process based on ion exchangers in fluidized bed. A flowsheet is given with main advantages resulted.« less
Advancing Performance Assessment for Disposal of Depleted Uranium at Clive Utah - 12493
DOE Office of Scientific and Technical Information (OSTI.GOV)
Black, Paul; Tauxe, John; Perona, Ralph
2012-07-01
A Performance Assessment (PA) for disposal of depleted uranium (DU) waste has recently been completed for a potential disposal facility at Clive in northwestern Utah. For the purposes of this PA, 'DU waste' includes uranium oxides of all naturally-occurring isotopes, though depleted in U-235, varying quantities of other radionuclides introduced to the uranium enrichment process in the form of used nuclear reactor fuel (reactor returns), and decay products of all of these radionuclides. The PA will be used by the State of Utah to inform an approval decision for disposal of DU waste at the facility, and will be availablemore » to federal regulators as they revisit rulemaking for the disposal of DU. The specific performance objectives of the Clive DU PA relate to annual individual radiation dose within a 10,000-year performance period, groundwater concentrations of specific radionuclides within a 500-year compliance period, and site stability in the longer term. Fate and transport processes that underlie the PA model include radioactive decay and ingrowth, diffusion in gaseous and water phases, water advection in unsaturated and saturated zones, transport caused by plant and animal activity, cover naturalization, natural and anthropogenic erosion, and air dispersion. Fate and transport models were used to support the dose assessment and the evaluation of groundwater concentrations. Exposure assessment was based on site-specific scenarios, since the traditional human exposure scenarios suggested by DOE and NRC guidance are unrealistic for this site. Because the U-238 in DU waste reaches peak radioactivity (secular equilibrium) after 2 million years (My) following its separation, the PA must also evaluate the impact of climate change cycles, including the return of pluvial lakes such as Lake Bonneville. The first draft of the PA has been submitted to the State of Utah for review. The results of this preliminary analysis indicate that doses are very low for the site-specific receptors for the 10,000-year compliance period. This is primarily because DU waste is not highly radioactive within this time frame, the DU waste is assumed to be buried beneath zones exposed by erosion, groundwater concentrations of DU waste constituents do not exceed groundwater protection limits with in the 500-year compliance period, and the first deep lake occurrence will disperse DU waste across a large area, and will ultimately be covered by lake-derived sediment. A probabilistic PA model was constructed that considered DU waste and decay product doses to site-specific receptors for a 10,000-yr performance period, as well as deep-time effects. The quantitative results are summarized in Table VII. Doses (as TEDE) are always less than 5 mSv in a year, and doses to the offsite receptors are always much less than 0.25 mSv in a year. Groundwater concentrations of Tc-99 are always less than its GWPL except when the Tc-99 contaminated waste is disposed below grade. Even in this case, the median groundwater concentration is only 4.18 Bq/L (113 pCi/L), which is more than one order of magnitude less than the GWPL for Tc-99. The results overall suggest that there are disposal configurations that can be used to dispose of the proposed quantities of DU waste that are adequately protective of human health. (authors)« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gates, Jacklyn M; Gates, J.M.; Garcia, M.A.
2008-01-15
Isotopes of rutherfordium (258-261Rf) were produced in irradiations of 238U targets with 26Mg beams. Excitation functions were measured for the 4n, 5n and 6n exit channels. Production of 261Rf in the 3n exit channel with a cross section of 28+92-26 pb was observed. Alpha decay of 258Rf was observed for the first time with an alpha-particle energy of 9.05+-0.03 MeV and an alpha/total decay branching ratio of 0.31+-0.11. In 259Rf, the electron capture/total decay branching ratio was measured to be 0.15+-0.04. The measured half-lives for 258Rf, 259Rf and 260Rf were 14.7+1.2-1.0 ms, 2.5+0.4-0.3 s and 22.2+3.0-2.4 ms, respectively, in agreementmore » with literature data. The systematics of the alpha decay Q values and of the partial spontaneous fission half-lives were evaluated for even-even nuclides in the region of the N = 152, Z = 100 deformed shell. The influence of the N = 152 shell on the alpha decay Q values for rutherfordium was observed to be similar to that of the lighter elements (96<_ Z<_ 102). However, the N = 152 shell does not stabilize the rutherfordium isotopes against spontaneous fission, as it does in the lighter elements (96<_ Z<_102).« less
Denton, J. S.; Goldstein, S. J.; Paviet, P.; ...
2016-04-10
Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca inmore » the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Furthermore, uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface.« less
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.
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.
222Rn emanation from uranium-glazed ceramics.
Biagioni, R N; Sheets, R W
2001-02-01
Orange-red uranium-glazed dinnerware was found to emanate 222Rn to produce an average of less than 0.1 Bq 222Rn decay per piece, which should have no associated health risks. Comparison of 222Rn emanation to 226Ra in glazes (measured by alpha spectrometry) indicated inefficient emanation (<5%) of 222Rn, consistent with the low radon levels observed and with the presence of 222Rn progeny in glazes. These studies also showed that reagent grade uranium compounds may emanate measurable 222Rn.
Thomas, P A; Gates, T E
1999-01-01
The richest uranium ore bodies ever discovered (Cigar Lake and McArthur River) are presently under development in northeastern Saskatchewan. This subarctic region is also home to several operating uranium mines and aboriginal communities, partly dependent upon caribou for subsistence. Because of concerns over mining impacts and the efficient transfer of airborne radionuclides through the lichen-caribou-human food chain, radionuclides were analyzed in tissues from 18 barren-ground caribou (Rangifer tarandus groenlandicus). Radionuclides included uranium (U), radium (226Ra), lead (210Pb), and polonium (210Po) from the uranium decay series; the fission product (137Cs) from fallout; and naturally occurring potassium (40K). Natural background radiation doses average 2-4 mSv/year from cosmic rays, external gamma rays, radon inhalation, and ingestion of food items. The ingestion of 210Po and 137Cs when caribou are consumed adds to these background doses. The dose increment was 0.85 mSv/year for adults who consumed 100 g of caribou meat per day and up to 1.7 mSv/year if one liver and 10 kidneys per year were also consumed. We discuss the cancer risk from these doses. Concentration ratios (CRs), relating caribou tissues to lichens or rumen (stomach) contents, were calculated to estimate food chain transfer. The CRs for caribou muscle ranged from 1 to 16% for U, 6 to 25% for 226Ra, 1 to 2% for 210Pb, 6 to 26% for 210Po, 260 to 370% for 137Cs, and 76 to 130% for 40K, with 137Cs biomagnifying by a factor of 3-4. These CRs are useful in predicting caribou meat concentrations from the lichens, measured in monitoring programs, for the future evaluation of uranium mining impacts on this critical food chain. Images Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 PMID:10378999
Xu, Yihong; Qiao, Jixin; Hou, Xiaolin; Pan, Shaoming; Roos, Per
2014-02-01
This paper reports an analytical method for the determination of plutonium isotopes ((238)Pu, (239)Pu, (240)Pu, (241)Pu) in environmental samples using anion exchange chromatography in combination with extraction chromatography for chemical separation of Pu. Both radiometric methods (liquid scintillation counting and alpha spectrometry) and inductively coupled plasma mass spectrometry (ICP-MS) were applied for the measurement of plutonium isotopes. The decontamination factors for uranium were significantly improved up to 7.5 × 10(5) for 20 g soil compared to the level reported in the literature, this is critical for the measurement of plutonium isotopes using mass spectrometric technique. Although the chemical yield of Pu in the entire procedure is about 55%, the analytical results of IAEA soil 6 and IAEA-367 in this work are in a good agreement with the values reported in the literature or reference values, revealing that the developed method for plutonium determination in environmental samples is reliable. The measurement results of (239+240)Pu by alpha spectrometry agreed very well with the sum of (239)Pu and (240)Pu measured by ICP-MS. ICP-MS can not only measure (239)Pu and (240)Pu separately but also (241)Pu. However, it is impossible to measure (238)Pu using ICP-MS in environmental samples even a decontamination factor as high as 10(6) for uranium was obtained by chemical separation. © 2013 Elsevier B.V. All rights reserved.
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
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.
Natural radioactivity and trace metals in crude oils: implication for health.
Ajayi, T R; Torto, N; Tchokossa, P; Akinlua, A
2009-02-01
Crude oil samples were collected from six different fields in the central Niger Delta in order to determine their natural radioactivity and trace element contents, with the aim of assessing the radiological health implications and environmental health hazard of the metals, and also to provide natural radioactivity baseline data that could be used for more comprehensive future study in this respect. The activity concentrations of the radionuclides were measured using a well, accurately calibrated and shielded vertical cryostat, Canberra coaxial high-purity germanium (HPGe) detector system, and the derived doses were evaluated. The metal concentrations were determined by the graphite furnace atomic absorption spectroscopic (GFAAS) method. The radionuclides identified with reliable regularity belong to the decay series of naturally occurring radionuclides headed by (238)U and (232)Th along with the non-decay series radionuclide, (40)K. The averaged activity concentrations obtained were 10.52 +/- 0.03 Bq kg(-1), 0.80 +/- 0.37 Bq kg(-1) and 0.17 +/- 0.09 Bq kg(-1) for (40)K, (238)U and (232)Th, respectively. The equivalent doses were very low, ranging from 0.0028 to 0.012 mSv year(-1) with a mean value of 0.0070 mSv year(-1). The results obtained were low, and hence, the radioactivity content from the crude oils in the Niger delta oil province of Nigeria do not constitute any health hazard to occupationally exposed workers, the public and the end user. The concentrations of the elements (As, Cd, Co, Fe, Mn, Ni, Se and V) determined ranged from 0.73 to 202.90 ppb with an average of 74.35 ppb for the oil samples analysed. The pattern of occurrence of each element agreed with the earlier studies from other parts of the Niger Delta. It was obvious from this study and previous ones that the Niger Delta oils have low metal contents. However, despite the low concentrations, they could still pose an intrinsic health hazard considering their cumulative effects in the environment. Also, various studies on the impact of oil spillage and activities of oil exploration and production on organisms in the immediate environment suggest this.
U-Sries Disequilibra in Soils, Pena Blanca Natural Analog, Chihuahua, Mexico
DOE Office of Scientific and Technical Information (OSTI.GOV)
D. French; E. Anthony; P. Goodell
2006-03-16
The Nopal I uranium deposit located in the Sierra Pena Blanca, Mexico. The deposit was mined in the early 1980s, and ore was stockpiled close by. This stockpile area was cleared and is now referred to as the Prior High Grade Stockpile (PHGS). Some of the high-grade boulders from the site rolled downhill when it was cleared in the 1990s. For this study soil samples were collected from the alluvium surrounding and underlying one of these boulders. A bulk sample of the boulder was also collected. Because the Prior High Grade Stockpile had no ore prior to the 1980s amore » maximum residence time for the boulder is about 25 years, this also means that the soil was at background as well. The purpose of this study is to characterize the transport of uranium series radionuclides from ore to the soil. Transport is characterized by determining the activities of individual radionuclides and daughter to parent ratios. Isotopes of the uranium series decay chain detected include {sup 210}Pb, {sup 234}U, {sup 230}Th, {sup 226}Ra, {sup 214}Pb, and {sup 214}Bi. Peak areas for each isotope are determined using gamma-ray spectroscopy with a Canberra Ge (Li) detector and GENIE 2000 software. The boulder sample is close to secular equilibrium when compared to the standard BL-5 (Beaver Lodge Uraninite from Canada). Results for the soils, however, indicate that some daughter/parent pairs are in secular disequilibrium. These daughter/parent (D/P) ratios include {sup 230}Th/{sup 234}U, which is greater than unity, {sup 226}Ra/{sup 230}Th, which is also greater than unity, and {sup 210}Pb/{sup 214}Bi, which is less than unity. The gamma-ray spectrum for organic material lacks {sup 230}Th peaks, but contains {sup 234}U and {sup 226}Ra, indicating that plants preferentially incorporate {sup 226}Ra. Our results, combined with previous studies require multistage history of mobilization of the uranium series radionuclides. Earlier studies at the ore zone could limit the time span for mobilization only to a few thousand years. The contribution of this study is that the short residence time of the ore at the Prior High Grade Stockpile requires a time span for mobilization of 20-30 years.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Weismann, J.; Young, C.; Masciulli, S.
2007-07-01
Lowry Air Force Base (Lowry) was closed in September 1994 as part of the Base Realignment and Closure (BRAC) program and the base was transferred to the Lowry Redevelopment Authority in 1995. As part of the due diligence activities conducted by the Air Force, a series of remedial investigations were conducted across the base. A closed waste landfill, designated Operable Unit 2 (OU 2), was initially assessed in a 1990 Remedial Investigation (RI; [1]). A Supplemental Remedial Investigation was conducted in 1995 [2] and additional studies were conducted in a 1998 Focused Feasibility Study. [3] The three studies indicated thatmore » gross alpha, gross beta, and uranium concentrations were consistently above regulatory standards and that there were detections of low concentrations other radionuclides. Results from previous investigations at OU 2 have shown elevated gross alpha, gross beta, and uranium concentrations in groundwater, surface water, and sediments. The US Air Force has sought to understand the provenance of these radionuclides in order to determine if they could be due to leachates from buried radioactive materials within the landfill or whether they are naturally-occurring. The Air Force and regulators agreed to use a one-year monitoring and sampling program to seek to explain the origins of the radionuclides. Over the course of the one-year program, dissolved uranium levels greater than the 30 {mu}g/L Maximum Contaminant Level (MCL) were consistently found in both up-gradient and down-gradient wells at OU 2. Elevated Gross Alpha and Gross Beta measurements that were observed during prior investigations and confirmed during the LTM were found to correlate with high dissolved uranium content in groundwater. If Gross Alpha values are corrected to exclude uranium and radon contributions in accordance with US EPA guidance, then the 15 pCi/L gross alpha level is not exceeded. The large dataset also allowed development of gross alpha to total uranium correlation factors so that gross alpha action levels can be applied to future long-term landfill monitoring to track radiological conditions at lower cost. Ratios of isotopic uranium results were calculated to test whether the elevated uranium displayed signatures indicative of military use. Results of all ratio testing strongly supports the conclusion that the uranium found in groundwater, surface water, and sediment at OU 2 is naturally-occurring and has not undergone anthropogenic enrichment or processing. U-234:U-238 ratios also show that a disequilibrium state, i.e., ratio greater than 1, exists throughout OU 2 which is indicative of long-term aqueous transport in aged aquifers. These results all support the conclusion that the elevated uranium observed at OU 2 is due to the high concentrations in the regional watershed. Based on the results of this monitoring program, we concluded that the elevated uranium concentrations measured in OU 2 groundwater, surface water, and sediment are due to the naturally-occurring uranium content of the regional watershed and are not the result of waste burials in the former landfill. Several lines of evidence indicate that natural uranium has been naturally concentrated beneath OU 2 in the geologic past and the higher of uranium concentrations in down-gradient wells is the result of geochemical processes and not the result of a uranium ore disposal. These results therefore provide the data necessary to support radiological closure of OU 2. (authors)« less
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.
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.
León Vintró, L; Mitchell, P I; Omarova, A; Burkitbayev, M; Jiménez Nápoles, H; Priest, N D
2009-04-01
New data are reported on the concentrations, isotopic composition and speciation of americium, plutonium and uranium in surface and ground waters in the Sarzhal region of the Semipalatinsk Test Site, and an adjacent area including the settlement of Sarzhal. The data relate to filtered water and suspended particulate from (a) streams originating in the Degelen Mountains, (b) the Tel'kem 1 and Tel'kem 2 atomic craters, and (c) wells on farms located within the study area and at Sarzhal. The measurements show that (241)Am, (239,240)Pu and (238)U concentrations in well waters within the study area are in the range 0.04-87mBq dm(-3), 0.7-99mBq dm(-3), and 74-213mBq dm(-3), respectively, and for (241)Am and (239,240)Pu are elevated above the levels expected solely on the basis of global fallout. Concentrations in streams sourced in the Degelen Mountains are similar, while concentrations in the two water-filled atomic craters are somewhat higher. Suspended particulate concentrations in well waters vary considerably, though median values are very low, at 0.01mBq dm(-3), 0.08mBq dm(-3) and 0.32mBq dm(-3) for (241)Am, (239,240)Pu and (238)U, respectively. The (235)U/(238)U isotopic ratio in almost all well and stream waters is slightly elevated above the 'best estimate' value for natural uranium worldwide, suggesting that some of the uranium in these waters is of test-site provenance. Redox analysis shows that on average most of the plutonium present in the microfiltered fraction of these waters is in a chemically reduced form (mean 69%; 95% confidence interval 53-85%). In the case of the atomic craters, the proportion is even higher. As expected, all of the americium present appears to be in a reduced form. Calculations suggest that annual committed effective doses to individual adults arising from the daily ingestion of these well waters are in the range 11-42microSv (mean 21microSv). Presently, the ground water feeding these wells would not appear to be contaminated with radioactivity from past underground testing in the Degelen Mountains or from the Tel'kem explosions.
NASA Astrophysics Data System (ADS)
Shimizu, Yohei; Kubo, Toshiyuki; Fukuda, Naoki; Inabe, Naohito; Kameda, Daisuke; Sato, Hiromi; Suzuki, Hiroshi; Takeda, Hiroyuki; Yoshida, Koichi; Lorusso, Giuseppe; Watanabe, Hiroshi; Simpson, Gary S.; Jungclaus, Andrea; Baba, Hidetada; Browne, Frank; Doornenbal, Pieter; Gey, Guillaunme; Isobe, Tadaaki; Li, Zhihuan; Nishimura, Shunji; Söderström, Pär-Anders; Sumikama, Toshiyuki; Taprogge, Jan; Vajta, Zsolt; Wu, Jin; Xu, Zhengyu; Odahara, Atsuko; Yagi, Ayumi; Nishibata, Hiroki; Lozeva, Radomira; Moon, Changbum; Jung, HyoSoon
2018-01-01
The search for new isotopes using the in-flight fission of a 238U beam has been conducted concurrently with decay measurements, during the so-called EURICA campaigns, at the RIKEN Nishina Center RI Beam Factory. Fission fragments were analyzed and identified in flight using the BigRIPS separator. We have identified the following 36 new neutron-rich isotopes: 104Rb, 113Zr, 116Nb, 118,119Mo, 121,122Tc, 125Ru, 127,128Rh, 129,130,131Pd, 132Ag, 134Cd, 136,137In, 139,140Sn, 141,142Sb, 144,145Te, 146,147I, 149,150Xe, 149,150,151Cs, 153,154Ba, and 154,155,156,157La.
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.
Measurement of the double- β decay half-life of 136 Xe with the KamLAND-Zen experiment
DOE Office of Scientific and Technical Information (OSTI.GOV)
Gando, A.; Gando, Y.; Hanakago, H.
2012-04-19
We present results from the KamLAND-Zen double-beta decay experiment based on an exposure of 77.6 days with 129 kg of 136Xe. The measured two-neutrino double-beta decay half-life of 136Xe is Tmore » $$2ν\\atop{1/2}$$ = 2.38 ± 0.02(stat) ± 0.14(syst) x10 21 yr, consistent with a recent measurement by EXO-200. We also obtain a lower limit for the neutrinoless double-beta decay half-life, T$$0ν\\atop{1/2}$$ > 5.7 x 10 24 yr at 90% C.L.« less
Method of fabricating a uranium-bearing foil
Gooch, Jackie G [Seymour, TN; DeMint, Amy L [Kingston, TN
2012-04-24
Methods of fabricating a uranium-bearing foil are described. The foil may be substantially pure uranium, or may be a uranium alloy such as a uranium-molybdenum alloy. The method typically includes a series of hot rolling operations on a cast plate material to form a thin sheet. These hot rolling operations are typically performed using a process where each pass reduces the thickness of the plate by a substantially constant percentage. The sheet is typically then annealed and then cooled. The process typically concludes with a series of cold rolling passes where each pass reduces the thickness of the plate by a substantially constant thickness amount to form the foil.
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.
Depleted uranium: an overview of its properties and health effects.
Shawky, S
2002-01-01
There has been much debate about the use of depleted uranium in the Gulf War and its health effects on United States and European war veterans. However, studies on the impact of this radioactive substance on the residents of the surrounding Gulf region are far from adequate. Depleted uranium introduces large quantities of radioactive material that is hazardous to biological organisms, continues to decay for millennia and is able to travel tens of kilometres in air. If depleted uranium were used in the Gulf War, its impact on the health of people in the area would have been considerable. This review of depleted uranium--its origin, properties, uses and effects on the human environment and health--aims to trigger further research on this subject.
Atomic Fuel, Understanding the Atom Series. Revised.
ERIC Educational Resources Information Center
Hogerton, John F.
This publication is part of the "Understanding the Atom" series. Complete sets of the series are available free to teachers, schools, and public librarians who can make them available for reference or use by groups. Among the topics discussed are: What Atomic Fuel Is; The Odyssey of Uranium; Production of Uranium; Fabrication of Reactor…
Studies of Plutonium-238 Production at the High Flux Isotope Reactor
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lastres, Oscar; Chandler, David; Jarrell, Joshua J
The High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) is a versatile 85 MW{sub th}, pressurized, light water-cooled and -moderated research reactor. The core consists of two fuel elements, an inner fuel element (IFE) and an outer fuel element (OFE), each constructed of involute fuel plates containing high-enriched-uranium (HEU) fuel ({approx}93 wt% {sup 235}U/U) in the form of U{sub 3}O{sub 8} in an Al matrix and encapsulated in Al-6061 clad. An over-moderated flux trap is located in the center of the core, a large beryllium reflector is located on the outside of the core, and two controlmore » elements (CE) are located between the fuel and the reflector. The flux trap and reflector house numerous experimental facilities which are used for isotope production, material irradiation, and cold/thermal neutron scattering. Over the past five decades, the US Department of Energy (DOE) and its agencies have been producing radioisotope power systems used by the National Aeronautics and Space Administration (NASA) for unmanned, long-term space exploration missions. Plutonium-238 is used to power Radioisotope Thermoelectric Generators (RTG) because it has a very long half-life (t{sub 1/2} {approx} 89 yr.) and it generates about 0.5 watts/gram when it decays via alpha emission. Due to the recent shortage and uncertainty of future production, the DOE has proposed a plan to the US Congress to produce {sup 238}Pu by irradiating {sup 237}Np as early as in fiscal year 2011. An annual production rate of 1.5 to 2.0 kg of {sup 238}Pu is expected to satisfy these needs and could be produced in existing national nuclear facilities like HFIR and the Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL). Reactors at the Savannah River Site were used in the past for {sup 238}Pu production but were shut down after the last production in 1988. The nation's {sup 237}Np inventory is currently stored at INL. A plan for producing {sup 238}Pu at US research reactor facilities such as the High Flux Isotope Reactor at ORNL has been initiated by the US DOE and NASA for space exploration needs. Two Monte Carlo-based depletion codes, TRITON (ORNL) and VESTA (IRSN), were used to study the {sup 238}Pu production rates with varying target configurations in a typical HFIR fuel cycle. Preliminary studies have shown that approximately 11 grams and within 15 to 17 grams of {sup 238}Pu could be produced in the first irradiation cycle in one small and one large VXF facility, respectively, when irradiating fresh target arrays as those herein described. Important to note is that in this study we discovered that small differences in assumptions could affect the production rates of Pu-238 observed. The exact flux at a specific target location can have a significant impact upon production, so any differences in how the control elements are modeled as a function of exposure, will also cause differences in production rates. In fact, the surface plot of the large VXF target Pu-238 production shown in Figure 3 illustrates that the pins closest to the core can potentially have production rates as high as 3 times those of pins away from the core, thus implying that a cycle-to-cycle rotation of the targets may be well advised. A methodology for generating spatially-dependent, multi-group self-shielded cross sections and flux files with the KENO and CENTRM codes has been created so that standalone ORIGEN-S inputs can be quickly constructed to perform a variety of {sup 238}Pu production scenarios, i.e. combinations of the number of arrays loaded and the number of irradiation cycles. The studies herein shown with VESTA and TRITON/KENO will be used to benchmark the standalone ORIGEN.« less
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.
Cook, Gordon T; MacKenzie, Angus B
2014-07-01
A review of information that can be provided from measurements made on natural and anthropogenic radionuclide activities in human skeletal remains has been undertaken to establish what reliable information of forensic anthropological use can be obtained regarding years of birth and death (and hence post-mortem interval (PMI)). Of the anthropogenic radionuclides that have entered the environment, radiocarbon ((14)C) can currently be used to generate the most useful and reliable information. Measurements on single bones can indicate whether or not the person died during the nuclear era, while recent research suggests that measurements on trabecular bone may, depending on the chronological age of the remains, provide estimates of year of death and hence PMI. Additionally, (14)C measurements made on different components of single teeth or on teeth formed at different times can provide estimates of year of birth to within 1-2 years of the true year. Of the other anthropogenic radionuclides, (90)Sr shows some promise but there are problems of (1) variations in activities between individuals, (2) relatively large analytical uncertainties and (3) diagenetic contamination. With respect to natural series radionuclides, it is concluded that there is no convincing evidence that (210)Pb dating can be used in a rigorous, quantitative fashion to establish a PMI. Similarly, for daughter/parent pairs such as (210)Po/(210)Pb (from the (238)U decay series) and (228)Th/(228)Ra (from the (232)Th decay series), the combination of analytical uncertainty and uncertainty in activity ratios at the point of death inevitably results in major uncertainty in any estimate of PMI. However, observation of the disequilibrium between these two daughter/parent pairs could potentially be used in a qualitative way to support other forensic evidence.
Depleted and natural uranium: chemistry and toxicological effects.
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.
NASA Astrophysics Data System (ADS)
Deschanels, X.; Seydoux-Guillaume, A. M.; Magnin, V.; Mesbah, A.; Tribet, M.; Moloney, M. P.; Serruys, Y.; Peuget, S.
2014-05-01
Zirconolite and monazite matrices are potential ceramics for the containment of actinides (Np, Cm, Am, Pu) which are produced over the reprocessing of spent nuclear fuel. Actinides decay mainly through the emission of alpha particles, which in turn causes most ceramics to undergo structural and textural changes (amorphization and/or swelling). In order to study the effects of alpha decays on the above mentioned ceramics two parallel approaches were set up. The first involved the use of an external irradiation source, Au, which allowed the deposited recoil energy to be simulated. The second was based on short-lived actinide doping with 238Pu, (i.e. an internal source), via the incorporation of plutonium oxide into both the monazite and zirconolite structures during synthesis. In both types of irradiation experiments, the zirconolite samples became amorphous at room temperature with damage close to 0.3 dpa; corresponding to a critical dose of 4 × 1018 α g-1 (i.e. ∼1.3 × 1021 keV cm-3). Both zirconolite samples also showed the same degree of macroscopic swelling at saturation (∼6%), with ballistic processes being the predominant damaging effect. In the case of the monazite however, the macroscopic swelling and amorphization were dependent on the nature of the irradiation. Externally, (Au), irradiated samples became amorphous while also demonstrating a saturation swelling of up to 8%. In contrast to this, the swelling of the 238Pu doped samples was much smaller at ∼1%. Also, unlike the externally (Au) irradiated monazite these 238Pu doped samples remained crystalline up to 7.5 × 1018 α g-1 (0.8 dpa). XRD, TEM and swelling measurements were used to fully characterize and interpret this behavior. The low swelling and the conservation of the crystalline state of 238Pu doped monazite samples indicates that alpha annealing took place within this material.
Neutrons as Party Animals: An Analogy for Understanding Heavy-Element Fissility
ERIC Educational Resources Information Center
Reed, B. Cameron
2012-01-01
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…
Uranium isotopes in groundwater occurring at Amazonas State, Brazil.
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.
NASA Astrophysics Data System (ADS)
De Vleeschouwer, David; Dunlea, Ann G.; Auer, Gerald; Anderson, Chloe H.; Brumsack, Hans; de Loach, Aaron; Gurnis, Michael C.; Huh, Youngsook; Ishiwa, Takeshige; Jang, Kwangchul; Kominz, Michelle A.; März, Christian; Schnetger, Bernhard; Murray, Richard W.; Pälike, Heiko; Expedition 356 shipboard scientists, IODP
2017-04-01
During International Ocean Discovery Program (IODP) expeditions, shipboard-generated data provide the first insights into the cored sequences. The natural gamma radiation (NGR) of the recovered material, for example, is routinely measured on the ocean drilling research vessel DV JOIDES Resolution. At present, only total NGR counts are readily available as shipboard data, although full NGR spectra (counts as a function of gamma-ray energy level) are produced and archived. These spectra contain unexploited information, as one can estimate the sedimentary contents of potassium (K), thorium (Th), and uranium (U) from the characteristic gamma-ray energies of isotopes in the 40K, 232Th, and 238U radioactive decay series. Dunlea et al. [2013] quantified K, Th and U contents in sediment from the South Pacific Gyre by integrating counts over specific energy levels of the NGR spectrum. However, the algorithm used in their study is unavailable to the wider scientific community due to commercial proprietary reasons. Here, we present a new MATLAB algorithm for the quantification of NGR spectra that is transparent and accessible to future NGR users. We demonstrate the algorithm's performance by comparing its results to shore-based inductively coupled plasma-mass spectrometry (ICP-MS), inductively coupled plasma-emission spectrometry (ICP-ES), and quantitative wavelength-dispersive X-ray fluorescence (XRF) analyses. Samples for these comparisons come from eleven sites (U1341, U1343, U1366-U1369, U1414, U1428-U1430, U1463) cored in two oceans during five expeditions. In short, our algorithm rapidly produces detailed high-quality information on sediment properties during IODP expeditions at no extra cost. Dunlea, A. G., R. W. Murray, R. N. Harris, M. A. Vasiliev, H. Evans, A. J. Spivack, and S. D'Hondt (2013), Assessment and use of NGR instrumentation on the JOIDES Resolution to quantify U, Th, and K concentrations in marine sediment, Scientific Drilling, 15, 57-63.
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.
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.
Analysis of the 2H-evaporator scale samples (HTF-17-56, -57)
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hay, M.; Coleman, C.; Diprete, D.
Savannah River National Laboratory analyzed scale samples from both the wall and cone sections of the 242-16H Evaporator prior to chemical cleaning. The samples were analyzed for uranium and plutonium isotopes required for a Nuclear Criticality Safety Assessment of the scale removal process. The analysis of the scale samples found the material to contain crystalline nitrated cancrinite and clarkeite. Samples from both the wall and cone contain depleted uranium. Uranium concentrations of 16.8 wt% 4.76 wt% were measured in the wall and cone samples, respectively. The ratio of plutonium isotopes in both samples is ~85% Pu-239 and ~15% Pu-238 bymore » mass and shows approximately the same 3.5 times higher concentration in the wall sample versus the cone sample as observed in the uranium concentrations. The mercury concentrations measured in the scale samples were higher than previously reported values. The wall sample contains 19.4 wt% mercury and the cone scale sample 11.4 wt% mercury. The results from the current scales samples show reasonable agreement with previous 242-16H Evaporator scale sample analysis; however, the uranium concentration in the current wall sample is substantially higher than previous measurements.« less
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.
NASA Astrophysics Data System (ADS)
Luo, S.; Ku, T.; Todd, V.; Murrell, M. T.; Dinsmoor, J. C.
2007-05-01
The Nopal I uranium ore deposit at Pena Blanca, Mexico, located at > 200 meters above the groundwater table, provides an ideal natural analog for quantifying the effectiveness of geological barrier for isolation of radioactive waste nuclides from reaching the human environments through ground water transport. To fulfill such natural analog studies, three wells (PB1, PB2, and PB3 respectively) were drilled at the site from the land surface down to the saturated groundwater zone and ground waters were collected from each of these wells through large- volume sampling/in-situ Mn-filter filtration for analyses of short-lived uranium/thorium-series radionuclides. Our measurements from PB1 show that the groundwater standing in the hole has much lower 222Rn activity than the freshly pumped groundwater. From this change in 222Rn activity, we estimate the residence time of groundwater in PB1 to be about 20 days. Our measurements also show that the activities of short-lived radioisotopes of Th (234Th), Ra (228Ra, 224Ra, 223Ra), Rn (222Rn), Pb (210Pb), and Po (210Po) in PB1, PB2, and PB3 are all significantly higher than those from the other wells near the Nopal I site. These high activities provide evidence for the enrichment of long-lived U and Ra isotopes in the groundwater as well as in the associated adsorbed phases on the fractured aquifer rocks underneath the ore deposit. Such enrichment suggests a rapid dissolution of U and Ra isotopes from the uranium ore deposit in the vadose zone and the subsequent migration to the groundwater underneath. A reactive transport model can be established to characterize the in-situ transport of radionuclides at the site. The observed change of 222Rn activity at PB1 also suggests that the measured high radioactivityies in ground waters from the site isare not an artifact of drilling operations. However, further studies are needed to assess if or to what extent the radionuclide migration is affected by the previous mining activities at the site.
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.
NASA Astrophysics Data System (ADS)
Stirling, Claudine H.; Halliday, Alex N.; Potter, Emma-Kate; Andersen, Morten B.; Zanda, Brigitte
2006-11-01
The short-lived nuclide 247Cm is produced by r-process nucleosynthesis. When the presolar nebula formed, 247Cm became isolated from r-process production and its abundance diminished as a result of radioactive decay. Given its short half-life of only ˜ 16 million years, 247Cm is presently extinct, but its former presence should be detectable as small variations in 235U/ 238U in primitive meteoritic material, provided Cm was chemically fractionated from U at the time these solid objects formed. The magnitude of U isotopic anomalies in meteorites can thus be used to elucidate the timing and character of the last r-process nucleosynthetic event for input into models describing the formation and evolution of the early solar system. Here we report coupled U isotopic determinations and Nd/U proxy measurements for Cm/U in a series of acid-etched leachates and mineral assemblages extracted from meteorites containing primitive phases expected to show strong Cm-U fractionations. Using multiple-collector ICPMS, we are able to determine 235U/ 238U with 2 σ analytical uncertainties of ± 1 epsilon (1 epsilon = 1 part in 10,000) on sample sizes consisting of < 3 ng of 238U and < 20 pg of 235U. A double-spiking procedure using a mixed 236U- 233U spike was employed to allow instrumental mass fractionation to be reliably corrected internally and at high precision. Uranium isotopic results for almost 40 different phases show no resolvable deviations in 235U/ 238U from the chondritic value, at the ˜ 1-2 epsilon level. These data supplement our previous observations for a suite of bulk meteorite samples [C.H. Stirling, A.N. Halliday, D. Porcelli, In search of live 247Cm in the early solar system, Geochim. Cosmochim. Acta 69 (2005) 1059-1071] and provide evidence for a solar system initial 247Cm/ 235U of < 8 × 10 - 5 . Such a low value is difficult to explain without a long time-scale of ˜ 2.3 × 10 8 years between the last actinide producing r-process event and the formation of the solar system. As such it is difficult to reconcile with a model of actinide production in the same r-process forming event as 182Hf with a half-life of 8.9 My [G.J. Wasserburg, M. Busso, R. Gallino, Abundances of actinides and short-lived nonactinides in the interstellar medium: Diverse supernova sources for the r-processes, Astrophys. J. 466 (1996) L109-L113]. The alternative models of 182Hf production via a neutron-rich fast s-process, occurring, for example, in the helium burning shell in a 25 solar mass star during explosive nucleosynthesis [G.J. Wasserburg, M. Busso, R. Gallino, Abundances of actinides and short-lived nonactinides in the interstellar medium: Diverse supernova sources for the r-processes, Astrophys. J. 466 (1996) L109-L113], or via a distinct r-process event that is separate from actinide production [G.J. Wasserburg, M. Busso, R. Gallino, K.M. Nollet, Short-lived nuclei in the early solar system: Possible AGB sources, Nucl. Phys. A (in press)], may provide a viable explanation. However, further studies are also required to assess the veracity of Cm-U systematics, which are critically dependent on the suitability of using Nd and the light rare earth elements (LREEs) as a chemical proxy for Cm.
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.
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.
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.
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.
General Purpose Heat Source Simulator
NASA Technical Reports Server (NTRS)
Emrich, William J., Jr.
2008-01-01
The General Purpose Heat Source (GPHS) project seeks to combine the development of an electrically heated, single GPHS module simulator with the evaluation of potential nuclear surface power systems. The simulator is designed to match the form, fit, and function of actual GPHS modules which normally generate heat through the radioactive decay of Pu238. The use of electrically heated modules rather than modules containing Pu238 facilitates the testing of the subsystems and systems without sacrificing the quantity and quality of the test data gathered. Current GPHS activities are centered on developing robust heater designs with sizes and weights which closely match those of actual Pu238 fueled GPHS blocks. Designs are being pursued which will allow operation up to 1100 C.
Experimental study of the β decay of the very neutron-rich nucleus Ge 85
Korgul, A.; Rykaczewski, Krzysztof Piotr; Grzywacz, Robert Kazimierz; ...
2017-04-04
The β -decay properties of the very neutron-rich nucleus 85Ge, produced in the proton-induced fission of 238U, were studied at the Holifield Radioactive Ion Beam Facility at Oak Ridge National Laboratory. The level scheme of 33 85As 52 populated in 85Geβ γ decay was reconstructed and compared to shell-model calculations. The investigation of the systematics of low-energy levels in N =52 isotones together with shell-model analysis allowed us to provide an estimate of the low-energy structure of the more exotic N =52 isotone 81Cu.
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.
Molten salt extraction of transuranic and reactive fission products from used uranium oxide fuel
Herrmann, Steven Douglas
2014-05-27
Used uranium oxide fuel is detoxified by extracting transuranic and reactive fission products into molten salt. By contacting declad and crushed used uranium oxide fuel with a molten halide salt containing a minor fraction of the respective uranium trihalide, transuranic and reactive fission products partition from the fuel to the molten salt phase, while uranium oxide and non-reactive, or noble metal, fission products remain in an insoluble solid phase. The salt is then separated from the fuel via draining and distillation. By this method, the bulk of the decay heat, fission poisoning capacity, and radiotoxicity are removed from the used fuel. The remaining radioactivity from the noble metal fission products in the detoxified fuel is primarily limited to soft beta emitters. The extracted transuranic and reactive fission products are amenable to existing technologies for group uranium/transuranic product recovery and fission product immobilization in engineered waste forms.
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.
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
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.
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.
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.
Periodic Table of Elements: Los Alamos National Laboratory
during the formation of the Earth (4.5 billion years old) has long since decayed away by now. However ) neutrons. Neptunium-237 is irradiated with neutrons to create 238Pu, an alpha emitter for radioisotope
DOE Office of Scientific and Technical Information (OSTI.GOV)
Conway, R.; Wade, M.; Tharp, T.
1994-12-31
The first remediation of an Environmental Restoration (ER) Project site at Sandia National Laboratories (SNL) was successfully conducted in May and June 1994 at Technical Area II. The removal action involved four Uranium Calibration Pits (UCPs) filled with radioactive or hazardous materials. The concrete culvert pits were used to test and calibrate borehole radiometric logging tools for uranium exploration. The removal action consisted of excavating and containerizing the pit contents and contaminated soil beneath the culverts, removing the four culverts, and backfilling the excavation. Each UCP removal had unique complexities. Sixty 208-L drums of solid radioactive waste and eight 208-Lmore » drums of liquid hazardous waste were generated during the VCM. Two of the concrete culverts will be disposed as radioactive waste and two as solid waste. Uranium-238 was detected in UCP-2 ore material at 746 pci/g, and at 59 pci/g in UCP-1 silica sand. UCP-4 was empty; sludge from UCP-3 contained 122 mg/L (ppm) chromium.« less
XPS and SIMS study of the surface and interface of aged C + implanted uranium
Donald, Scott B.; Siekhaus, Wigbert J.; Nelson, Art J.
2016-09-08
X-ray photoelectron spectroscopy in combination with secondary ion mass spectrometry depth profiling were used to investigate the surface and interfacial chemistry of C + ion implanted polycrystalline uranium subsequently oxidized in air for over 10 years at ambient temperature. The original implantation of 33 keV C + ions into U 238 with a dose of 4.3 × 10 17 cm –3 produced a physically and chemically modified surface layer that was characterized and shown to initially prevent air oxidation and corrosion of the uranium after 1 year in air at ambient temperature. The aging of the surface and interfacial layersmore » were examined by using the chemical shift of the U 4f, C 1s, and O 1s photoelectron lines. In addition, valence band spectra were used to explore the electronic structure of the aged carbide surface and interface layer. Moreover, the time-of-flight secondary ion mass spectrometry depth profiling results for the aged sample confirmed an oxidized uranium carbide layer over the carbide layer/U metal interface.« less
Warnery, E; Ielsch, G; Lajaunie, C; Cale, E; Wackernagel, H; Debayle, C; Guillevic, J
2015-01-01
Terrestrial gamma dose rates show important spatial variations in France. Previous studies resulted in maps of arithmetic means of indoor terrestrial gamma dose rates by "departement" (French district). However, numerous areas could not be characterized due to the lack of data. The aim of our work was to obtain more precise estimates of the spatial variability of indoor terrestrial gamma dose rates in France by using a more recent and complete data base and geostatistics. The study was based on the exploitation of 97,595 measurements results distributed in 17,404 locations covering all of France. Measurements were done by the Institute for Radioprotection and Nuclear Safety (IRSN) using RPL (Radio Photo Luminescent) dosimeters, exposed during several months between years 2011 and 2012 in French dentist surgeries and veterinary clinics. The data used came from dosimeters which were not exposed to anthropic sources. After removing the cosmic rays contribution in order to study only the telluric gamma radiation, it was decided to work with the arithmetic means of the time-series measurements, weighted by the time-exposure of the dosimeters, for each location. The values varied between 13 and 349 nSv/h, with an arithmetic mean of 76 nSv/h. The observed statistical distribution of the gamma dose rates was skewed to the right. Firstly, ordinary kriging was performed in order to predict the gamma dose rate on cells of 1*1 km(2), all over the domain. The second step of the study was to use an auxiliary variable in estimates. The IRSN achieved in 2010 a classification of the French geological formations, characterizing their uranium potential on the bases of geology and local measurement results of rocks uranium content. This information is georeferenced in a map at the scale 1:1,000,000. The geological uranium potential (GUP) was classified in 5 qualitative categories. As telluric gamma rays mostly come from the progenies of the (238)Uranium series present in rocks, this information, which is exhaustive throughout France, could help in estimating the telluric gamma dose rates. Such an approach is possible using multivariate geostatistics and cokriging. Multi-collocated cokriging has been performed on 1*1 km(2) cells over the domain. This model used gamma dose rate measurement results and GUP classes. Our results provide useful information on the variability of the natural terrestrial gamma radiation in France ('natural background') and exposure data for epidemiological studies and risk assessment from low dose chronic exposures. Copyright © 2014 Elsevier Ltd. All rights reserved.
Results of the Excreta Bioassay Quality Control Program for April 1, 2009 through March 31, 2010
DOE Office of Scientific and Technical Information (OSTI.GOV)
Antonio, Cheryl L.
2012-07-19
A total of 58 urine samples and 10 fecal samples were submitted during the report period (April 1, 2009 through March 31, 2010) to General Engineering Laboratories, South Carolina by the Hanford Internal Dosimetry Program (IDP) to check the accuracy, precision, and detection levels of their analyses. Urine analyses for Sr, 238Pu, 239Pu, 241Am, 243Am 235U, 238U, elemental uranium and fecal analyses for 241Am, 238Pu and 239Pu were tested this year as well as four tissue samples for 238Pu, 239Pu, 241Am and 241Pu. The number of QC urine samples submitted during the report period represented 1.3% of the total samplesmore » submitted. In addition to the samples provided by IDP, GEL was also required to conduct their own QC program, and submit the results of analyses to IDP. About 33% of the analyses processed by GEL during the third year of this contract were quality control samples. GEL tested the performance of 21 radioisotopes, all of which met or exceeded the specifications in the Statement of Work within statistical uncertainty (Table 4).« less
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.
Lauer, Nancy; Vengosh, Avner; Dai, Shifeng
2017-11-21
Most coals in China have uranium concentrations up to 3 ppm, yet several coal deposits are known to be enriched in uranium. Naturally occurring radioactive materials (NORM) in these U-rich coals and associated coal combustion residues (CCRs) have not been well characterized. Here we measure NORM (Th, U, 228 Ra, 226 Ra, and 210 Pb) in coals from eight U-rich coal deposits in China and the associated CCRs from one of these deposits. We compared NORM in these U-rich coals and associated CCRs to CCRs collected from the Beijing area and natural loess sediments from northeastern China. We found elevated U concentrations (up to 476 ppm) that correspond to low 232 Th/ 238 U and 228 Ra/ 226 Ra activity ratios (≪1) in the coal samples. 226 Ra and 228 Ra activities correlate with 238 U and 232 Th activities, respectively, and 226 Ra activities correlate well with 210 Pb activities across all coal samples. We used measured NORM activities and ash yields in coals to model the activities of CCRs from all U-rich coals analyzed in this study. The activities of measured and modeled CCRs derived from U-rich coals exceed the standards for radiation in building materials, particularly for CCRs originating from coals with U > 10 ppm. Since beneficial use of high-U Chinese CCRs in building materials is not a suitable option, careful consideration needs to be taken to limit potential air and water contamination upon disposal of U- and Ra-rich CCRs.
Study of uranium oxidation states in geological material.
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.
Measurement of activation of helium gas by 238U beam irradiation at about 11 A MeV
NASA Astrophysics Data System (ADS)
Akashio, A.; Tanaka, K.; Imao, H.; Uwamino, Y.
2017-09-01
A new helium-gas stripper system has been applied at the 11 A MeV uranium beam of the Radioactive Isotope Beam Factory of the RIKEN accelerator facility. Although the gas stripper is important for the heavy-ion accelerator facility, the residual radiation that is generated is a serious problem for maintenance work. The residual dose was evaluated by using three-layered activation samples of aluminium and bismuth. The γ-rays from produced radionuclides with in-flight fission of the 238U beam and from the material of the chamber activated by neutrons were observed by using a Ge detector and compared with the values calculated by using the Monte-Carlo simulation code PHITS.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Perez-Sanchez, Danyl
As a result of a pilot project developed at the old Spanish 'Junta de Energia Nuclear' to extract uranium from ores, tailings materials were generated. Most of these residual materials were sent back to different uranium mines, but a small amount of it was mixed with conventional building materials and deposited near the old plant until the surrounding ground was flattened. The affected land is included in an area under institutional control and used as recreational area. At the time of processing, uranium isotopes were separated but other radionuclides of the uranium decay series as Th-230, Ra-226 and daughters remainmore » in the residue. Recently, the analyses of samples taken at different ground's depths confirmed their presence. This paper presents the methodology used to calculate the derived concentration level to ensure that the reference dose level of 0.1 mSv y-1 used as radiological criteria. In this study, a radiological impact assessment was performed modeling the area as recreational scenario. The modelization study was carried out with the code RESRAD considering as exposure pathways, external irradiation, inadvertent ingestion of soil, inhalation of resuspended particles, and inhalation of radon (Rn-222). As result was concluded that, if the concentration of Ra-226 in the first 15 cm of soil is lower than, 0.34 Bq g{sup -1}, the dose would not exceed the reference dose. Applying this value as a derived concentration level and comparing with the results of measurements on the ground, some areas with a concentration of activity slightly higher than latter were found. In these zones the remediation proposal has been to cover with a layer of 15 cm of clean material. This action represents a reduction of 85% of the dose and ensures compliance with the reference dose. (authors)« less
Wind Transport of Radionuclide- Bearing Dust, Peña Blanca, Chihuahua, Mexico
NASA Astrophysics Data System (ADS)
Velarde, R.; Goodell, P. C.; Gill, T. E.; Arimoto, R.
2007-05-01
This investigation evaluates radionuclide fractionation during wind erosion of high-grade uranium ore storage piles at Peña Blanca (50km north of Chihuahua City), Chihuahua, Mexico. The aridity of the local environment promotes dust resuspension by high winds. Although active operations ceased in 1983, the Peña Blanca mining district is one of Mexico`s most important uranium ore reserves. The study site contains piles of high grade ore, left loose on the surface, and separated by the specific deposits from which they were derived (Margaritas, Nopal I, and Puerto I). Similar locations do not exist in the United States, since uranium mining sites in the USA have been reclaimed. The Peña Blanca site serves as an analog for the Yucca Mountain project. Dust deposition is collected at Peña Blanca with BSNE sediment catchers (Fryrear, 1986) and marble dust traps (Reheis, 1999). These devices capture windblown sediment; subsequently, the sample data will help quantify potentially radioactive short term field sediment loss from the repository surface and determine sediment flux. Aerosols and surface materials will be analyzed and radioactivity levels established utilizing techniques such as gamma spectroscopy. As a result, we will be able to estimate how much radionuclide contaminated dust is being transported or attached geochemically to fine grain soils or minerals (e.g., clays or iron oxides). The high-grade uranium-bearing material is at secular equilibrium, thus the entire decay series is present. Of resulting interest is not only the aeolian transport of uranium, but also of the other daughter products. These studies will improve our understanding of geochemical cycling of radionuclides with respect to sources, transport, and deposition. The results may also have important implications for the geosciences and homeland security, and potential applications to public health. Funding for this project is provided in part via a NSF grant to Arimoto.
Update of the α - n Yields for Reactor Fuel Materials for the Interest of Nuclear Safeguards
NASA Astrophysics Data System (ADS)
Simakov, S. P.; van den Berg, Q. Y.
2017-01-01
The neutron yields caused by spontaneous α-decay of actinides and subsequent (α,xn) reactions were re-evaluated for the reactor fuel materials UO2, UF6, PuO2 and PuF4. For this purpose, the most recent reference data for decay parameters, α-particle stopping powers and (α,xn) cross sections were collected, analysed and used in calculations. The input data and elaborated code were validated against available thick target neutron yields in pure and compound materials measured at accelerators or with radioactive sources. This paper provides the specific neutron yields and their uncertainties resultant from α-decay of actinides 241Am, 249Bk, 252Cf, 242,244Cm, 237Np, 238-242Pu, 232Th and 232-236,238U in oxide and fluoride compounds. The obtained results are an update of previous reference tables issued by the Los Alamos National Laboratory in 1991 which were used for the safeguarding of radioactive materials by passive non-destructive techniques. The comparison of the updated values with previous ones shows an agreement within one estimated uncertainty (≈ 10%) for oxides, and deviations of up to 50% for fluorides.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Peters, William A; Smith, Michael Scott; Clement, Ryan
2013-10-01
The goal of this proposal is to enable neutron detection for precision Non-Destructive Assays (NDAs) of actinide-fluoride samples. Neutrons are continuously generated from a UFx matrix in a container or sample as a result of the interaction of alpha particles from uranium-decay α particles with fluorine nuclei in the matrix. Neutrons from 19F(α,n)22Na were once considered a poorly characterized background for assays of UFx samples via 238U spontaneous fission neutron detection [SMI2010B]. However, the yield of decay-α-driven neutrons is critical for 234,235U LEU and HEU assays, as it can used to determine both the total amount of uranium and themore » enrichment [BER2010]. This approach can be extremely valuable in a variety of safeguard applications, such as cylinder monitoring in underground uranium storage facilities, nuclear criticality safety studies, nuclear materials accounting, and other nonproliferation applications. The success of neutron-based assays critically depends on an accurate knowledge of the cross section of the (α,n) reaction that generates the neutrons. The 40% uncertainty in the 19F(α,n)22Na cross section currently limits the precision of such assays, and has been identified as a key factor in preventing accurate enrichment determinations [CRO2003]. The need for higher quality cross section data for (α,n) reactions has been a recurring conclusion in reviews of the nuclear data needs to support safeguards. The overarching goal of this project is to enable neutron detection to be used for precision Non- Destructive Assays (NDAs) of actinide-fluoride samples. This will significantly advance safeguards verification at existing declared facilities, nuclear materials accounting, process control, nuclear criticality safety monitoring, and a variety of other nonproliferation applications. To reach this goal, Idaho National Laboratory (INL), in partnership with Oak Ridge National Laboratory (ORNL), Rutgers University (RU), and the University of Notre Dame (UND), will focus on three specific items: (1) making a precision (better than 10 %) determination of the absolute cross section of the 19F(α,n)22Na reaction as a function of energy; (2) determining the spectrum of neutrons and γ-rays emitted from 19F(α,n)22Na over an energy range pertinent to NDA; and (3) performing simulations with this new cross section to extract the neutron yield (neutrons/gram/second) and resulting neutron- and gamma ray-spectra when α particles interact with fluorine nuclei in actinide samples, to aid in the design and reduce uncertainty of future NDA measurements and simulations.« less
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
P. R. Fresquez, D. C. Keller, C. D. Hathcock
2007-11-30
The Dual-Axis Radiographic Hydrodynamic Test (DARHT) Facility Mitigation Action Plan specifies the comparison of baseline conditions in biotic and abiotic media with those collected after operations have started. Operations at DARHT at Los Alamos National Laboratory started in 2000. In this study, the abundance and composition of birds collected near the DARHT facility from 2003 through 2006 were determined and compared to a preoperational period (1999). In addition, the levels of radionuclides and other inorganic chemicals in birds were compared to regional statistical reference levels (RSRLs). The number and diversity of bird species generally increased over preoperational levels with themore » greatest number of birds (412) and species (46) occurring in 2005. The most common bird species collected regardless of time periods were the chipping sparrow (Spizella passerina), the Virginia's warbler (Vermivora virginiae), the western bluebird (Sialia mexicana), the broad-tailed hummingbird (Selasphorus platycercus), the sage sparrow (Amphispiza belli), and the western tanager (Piranga ludoviciana). Most radionuclides, with the exception of uranium-234 and uranium-238, in (whole body) birds collected after operations began were either not detected or below RSRLs. Uranium-234 and uranium-238 concentrations in a few samples were far below screening levels and do not pose a potential unacceptable dose to the birds. In contrast, many inorganic chemicals, particularly arsenic and silver, in birds collected before and after operations began were in higher concentrations than RSRLs. Because birds (skin plus feathers) collected in the years before operations began contained higher levels of arsenic and silver than RSRLs and because there was no evidence of these metals in soil and sediment directly around the DARHT facility, the elevated levels of these metals in birds during early operations are probably not related to DARHT operations. Arsenic and silver in birds, however, have decreased over time to near background levels in 2007.« less
Hashimoto, Tetsuo; Sanada, Yukihisa; Uezu, Yasuhiro
2004-05-01
A delayed coincidence method, time-interval analysis (TIA), has been applied to successive alpha- alpha decay events on the millisecond time-scale. Such decay events are part of the (220)Rn-->(216)Po ( T(1/2) 145 ms) (Th-series) and (219)Rn-->(215)Po ( T(1/2) 1.78 ms) (Ac-series). By using TIA in addition to measurement of (226)Ra (U-series) from alpha-spectrometry by liquid scintillation counting (LSC), two natural decay series could be identified and separated. The TIA detection efficiency was improved by using the pulse-shape discrimination technique (PSD) to reject beta-pulses, by solvent extraction of Ra combined with simple chemical separation, and by purging the scintillation solution with dry N(2) gas. The U- and Th-series together with the Ac-series were determined, respectively, from alpha spectra and TIA carried out immediately after Ra-extraction. Using the (221)Fr-->(217)At ( T(1/2) 32.3 ms) decay process as a tracer, overall yields were estimated from application of TIA to the (225)Ra (Np-decay series) at the time of maximum growth. The present method has proven useful for simultaneous determination of three radioactive decay series in environmental samples.
[Analysis of the natural radioactivity due to the radon gas in the underground of Rome].
Magrini, A; Grana, M; Gianello, G; La Bua, R; Laurini, C; Messina, A; Pagliari, E; Bergamaschi, A
2007-01-01
Radon is a decay product of 238Uranium which is classified by WHO/IARC as group 1 carcinogen, given its causal relationship with lung neoplasia. An annual concentration of this gas higher than 500 Bq/m3 in workplace is considered potentially dangerous by the italian legislation. No data are currently available on radon level in underground tunnels, which are a potentially important source of exposure both for workers and travellers. Measurements have been performed in a station and within the trains. Two months integrated measures, and 5 days continuous (hourly) assessments have been performed. Integrated measurements have been performed by means of 12 passive dosimeters, containing a detector made of CR39 (polymeric type), whereas active scintillation-type dosimeters have been employed for continuous assessments. Two months integrated measures: radon level in the station was 665 +/- 71 Bq/m3, whereas values within the trains ranged between 96 and 117 Bq/m3. Continuous measurements: Mean radon level during work activities was 783 +/- 536 Bq/m3 and thereafter it rose to 850 +/- 131 Bq/m3 Radon nelle levels in underground tunnels may exceed attention levels, whereas within trains they remain well below these levels. Further studies focused to assess the risk of underground employers are needed.
Beta-Decay Rates for Exotic Nuclei and R-Process Nucleosynthesis
NASA Astrophysics Data System (ADS)
Suzuki, Toshio; Yoshida, Takashi; Wanajo, Shinya; Kajino, Toshitaka; Otsuka, Takaharu
Beta-decay rates for exotic nuclei at N = 126 relevant to r-process nucleosynthesis are studied by shell-model calculations. The half-lives obtained are used to study r-process nucleosynthesis in core-collapse supernova explosions and binary neutron star mergers. The element abundances are obtained up to the third peak as well as beyond the peak region up to uranium.
Fons, J; Zapata-García, D; Tent, J; Llauradó, M
2013-11-01
The determination of gross alpha, gross beta and (226)Ra activity in natural waters is useful in a wide range of environmental studies. Furthermore, gross alpha and gross beta parameters are included in international legislation on the quality of drinking water [Council Directive 98/83/EC]. In this work, a low-background liquid scintillation counter (Wallac, Quantulus 1220) was used to simultaneously determine gross alpha, gross beta and (226)Ra activity in natural water samples. Sample preparation involved evaporation to remove (222)Rn and its short-lived decay daughters. The evaporation process concentrated the sample ten-fold. Afterwards, a sample aliquot of 8 mL was mixed with 12 mL of Ultima Gold AB scintillation cocktail in low-diffusion vials. In this study, a theoretical mathematical model based on secular equilibrium conditions between (226)Ra and its short-lived decay daughters is presented. The proposed model makes it possible to determine (226)Ra activity from two measurements. These measurements also allow determining gross alpha and gross beta simultaneously. To validate the proposed model, spiked samples with different activity levels for each parameter were analysed. Additionally, to evaluate the model's applicability in natural water, eight natural water samples from different parts of Spain were analysed. The eight natural water samples were also characterised by alpha spectrometry for the naturally occurring isotopes of uranium ((234)U, (235)U and (238)U), radium ((224)Ra and (226)Ra), (210)Po and (232)Th. The results for gross alpha and (226)Ra activity were compared with alpha spectrometry characterization, and an acceptable concordance was obtained. Copyright © 2013 Elsevier Ltd. All rights reserved.
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.
Hinck, Jo E.; Linder, Greg L.; Finger, Susan E.; Little, Edward E.; Tillitt, Donald E.; Kuhne, Wendy
2010-01-01
This chapter compiles available chemical and radiation toxicity information for plants and animals from the scientific literature on naturally occurring uranium and associated radionuclides. Specifically, chemical and radiation hazards associated with radionuclides in the uranium decay series including uranium, thallium, thorium, bismuth, radium, radon, protactinium, polonium, actinium, and francium were the focus of the literature compilation. In addition, exposure pathways and a food web specific to the segregation areas were developed. Major biological exposure pathways considered were ingestion, inhalation, absorption, and bioaccumulation, and biota categories included microbes, invertebrates, plants, fishes, amphibians, reptiles, birds, and mammals. These data were developed for incorporation into a risk assessment to be conducted as part of an environmental impact statement for the Bureau of Land Management, which would identify representative plants and animals and their relative sensitivities to exposure of uranium and associated radionuclides. This chapter provides pertinent information to aid in the development of such an ecological risk assessment but does not estimate or derive guidance thresholds for radionuclides associated with uranium. Previous studies have not attempted to quantify the risks to biota caused directly by the chemical or radiation releases at uranium mining sites, although some information is available for uranium mill tailings and uranium mine closure activities. Research into the biological impacts of uranium exposure is strongly biased towards human health and exposure related to enriched or depleted uranium associated with the nuclear energy industry rather than naturally occurring uranium associated with uranium mining. Nevertheless, studies have reported that uranium and other radionuclides can affect the survival, growth, and reproduction of plants and animals. Exposure to chemical and radiation hazards is influenced by a plant’s or an animal’s life history and surrounding environment. Various species of plants, invertebrates, fishes, amphibians, reptiles, birds, and mammals found in the segregation areas that are considered species of concern by State and Federal agencies were included in the development of the site-specific food web. The utilization of subterranean habitats (burrows in uranium-rich areas, burrows in waste rock piles or reclaimed mining areas, mine tunnels) in the seasonally variable but consistently hot, arid environment is of particular concern in the segregation areas. Certain species of reptiles, amphibians, birds, and mammals in the segregation areas spend significant amounts of time in burrows where they can inhale or ingest uranium and other radionuclides through digging, eating, preening, and hibernating. Herbivores may also be exposed though the ingestion of radionuclides that have been aerially deposited on vegetation. Measured tissues concentrations of uranium and other radionuclides are not available for any species of concern in the segregation areas. The sensitivity of these animals to uranium exposure is unknown based on the existing scientific literature, and species-specific uranium presumptive effects levels were only available for two endangered fish species known to inhabit the segregation areas. Overall, the chemical toxicity data available for biological receptors of concern were limited, although chemical and radiation toxicity guidance values are available from several sources. However, caution should be used when directly applying these values to northern Arizona given the unique habitat and life history strategies of biological receptors in the segregation areas and the fact that some guidance values are based on models rather than empirical (laboratory or field) data. No chemical toxicity information based on empirical data is available for reptiles, birds, or wild mammals; therefore, the risks associated with uranium and other radionuclides are unknown for these biota.
(234)U/(238)U signatures associated with uranium ore bodies: part 1 Ranger 3.
Lowson, Richard T; McIntyre, Mark G
2013-04-01
The Ranger 3 ore body is an early Proterozoic U ore body in the Alligator Rivers U province, Northern Territory, Australia. It has surface expression with a redox front located between 30 and 50 m below the surface. The ground water U concentration and (234)U/(238)U AR signature in the top 10 m of the weathered zone are reported for 357 samples collected over 4 wet seasons, at 5 depths, along a transect in-line with the hydraulic gradient and along the centre line of the ore body and its associated dispersion halo. The results show that the weathered zone displays a general U isotope feature for this type of ore body with the (234)U/(238)U AR for the ground water and amorphous phase of the solid matrix being less than 1. The ground water (234)U/(238)U AR is independent of the annual monsoonal climate and depth within the range surface to 10 m. In the vicinity of the U ore body the ground water (234)U/(238)U AR is 0.75 and is very similar to the (234)U/(238)U AR of the amorphous phase of the solid (0.76). The (234)U/(238)U ARs of the amorphous phase and ground water rise and separate to values of 0.88 and 1.02 at the end of the transect. The rise and separation in (234)U/(238)U AR are interpreted as evidence that the source of the U in the ground water is from the water-soluble sub-phase of the amorphous phase and that the ground water flow is too fast to allow the processes occurring across the solid-water interface to reach chemical equilibrium. The data set is a robust characterisation of the coarse and fine detail of the (234)U/(238)U AR signature in the weathered zone of U ore bodies. Copyright © 2012 Elsevier Ltd. All rights reserved.
Irradiation of organic matter by uranium decay in the Alum Shale, Sweden
NASA Astrophysics Data System (ADS)
Lewan, M. D.; Buchardt, B.
1989-06-01
The Alum Shale of Sweden contains black shales with anomalously high uranium concentrations in excess of 100 ppm. Syngenetic or early diagenetic origin of this uranium indicates that organic matter within these shales has been irradiated by decaying uranium for approximately 500 Ma. Radiation-induced polymerization of alkanes through a free-radical cross-linking mechanism appears to be responsible for major alterations within the irradiated organic matter. Specific radiation-induced alterations include generation of condensate-like oils at reduced yields from hydrous pyrolysis experiments, decrease in atomic H/C ratios of kerogens, decrease in bitumen/organic-carbon ratios, and a relative increase in low-molecular weight triaromatic steroid hydrocarbons. Conversely, stable carbon isotopes of kerogens, reflectance of vitrinite-like macerais, oil-generation kinetics, and isomerization of 20R to 20S αα C 29-steranes were not affected by radiation. The radiation dosage needed to cause the alterations observed in the Alum Shale has been estimated to be in excess of 10 5 Mrads with respect to organic carbon. This value is used to estimate the potential for radiation damage to thermally immature organic matter in black shales through the geological rock record. High potential for radiation damage is not likely in Cenozoic and Mesozoic black shales but becomes more likely in lower Paleozoic and Precambrian black shales.
Radiochronological Age of a Uranium Metal Sample from an Abandoned Facility
DOE Office of Scientific and Technical Information (OSTI.GOV)
Meyers, L A; Williams, R W; Glover, S E
2012-03-16
A piece of scrap uranium metal bar buried in the dirt floor of an old, abandoned metal rolling mill was analyzed using multi-collector inductively coupled plasma mass spectroscopy (MC-ICP-MS). The mill rolled uranium rods in the 1940s and 1950s. Samples of the contaminated dirt in which the bar was buried were also analyzed. The isotopic composition of uranium in the bar and dirt samples were both the same as natural uranium, though a few samples of dirt also contained recycled uranium; likely a result of contamination with other material rolled at the mill. The time elapsed since the uranium metalmore » bar was last purified can be determined by the in-growth of the isotope {sup 230}Th from the decay of {sup 234}U, assuming that only uranium isotopes were present in the bar after purification. The age of the metal bar was determined to be 61 years at the time of this analysis and corresponds to a purification date of July 1950 {+-} 1.5 years.« less
Decay heat uncertainty quantification of MYRRHA
NASA Astrophysics Data System (ADS)
Fiorito, Luca; Buss, Oliver; Hoefer, Axel; Stankovskiy, Alexey; Eynde, Gert Van den
2017-09-01
MYRRHA is a lead-bismuth cooled MOX-fueled accelerator driven system (ADS) currently in the design phase at SCK·CEN in Belgium. The correct evaluation of the decay heat and of its uncertainty level is very important for the safety demonstration of the reactor. In the first part of this work we assessed the decay heat released by the MYRRHA core using the ALEPH-2 burnup code. The second part of the study focused on the nuclear data uncertainty and covariance propagation to the MYRRHA decay heat. Radioactive decay data, independent fission yield and cross section uncertainties/covariances were propagated using two nuclear data sampling codes, namely NUDUNA and SANDY. According to the results, 238U cross sections and fission yield data are the largest contributors to the MYRRHA decay heat uncertainty. The calculated uncertainty values are deemed acceptable from the safety point of view as they are well within the available regulatory limits.
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.
Illicit Trafficking of Natural Radionuclides
DOE Office of Scientific and Technical Information (OSTI.GOV)
Friedrich, Steinhaeusler; Lyudmila, Zaitseva
2008-08-07
Natural radionuclides have been subject to trafficking worldwide, involving natural uranium ore (U 238), processed uranium (yellow cake), low enriched uranium (<20% U 235) or highly enriched uranium (>20% U 235), radium (Ra 226), polonium (Po 210), and natural thorium ore (Th 232). An important prerequisite to successful illicit trafficking activities is access to a suitable logistical infrastructure enabling an undercover shipment of radioactive materials and, in case of trafficking natural uranium or thorium ore, capable of transporting large volumes of material. Covert en route diversion of an authorised uranium transport, together with covert diversion of uranium concentrate from anmore » operating or closed uranium mines or mills, are subject of case studies. Such cases, involving Israel, Iran, Pakistan and Libya, have been analyzed in terms of international actors involved and methods deployed. Using international incident data contained in the Database on Nuclear Smuggling, Theft and Orphan Radiation Sources (DSTO) and international experience gained from the fight against drug trafficking, a generic Trafficking Pathway Model (TPM) is developed for trafficking of natural radionuclides. The TPM covers the complete trafficking cycle, ranging from material diversion, covert material transport, material concealment, and all associated operational procedures. The model subdivides the trafficking cycle into five phases: (1) Material diversion by insider(s) or initiation by outsider(s); (2) Covert transport; (3) Material brokerage; (4) Material sale; (5) Material delivery. An Action Plan is recommended, addressing the strengthening of the national infrastructure for material protection and accounting, development of higher standards of good governance, and needs for improving the control system deployed by customs, border guards and security forces.« less
Illicit Trafficking of Natural Radionuclides
NASA Astrophysics Data System (ADS)
Friedrich, Steinhäusler; Lyudmila, Zaitseva
2008-08-01
Natural radionuclides have been subject to trafficking worldwide, involving natural uranium ore (U 238), processed uranium (yellow cake), low enriched uranium (<20% U 235) or highly enriched uranium (>20% U 235), radium (Ra 226), polonium (Po 210), and natural thorium ore (Th 232). An important prerequisite to successful illicit trafficking activities is access to a suitable logistical infrastructure enabling an undercover shipment of radioactive materials and, in case of trafficking natural uranium or thorium ore, capable of transporting large volumes of material. Covert en route diversion of an authorised uranium transport, together with covert diversion of uranium concentrate from an operating or closed uranium mines or mills, are subject of case studies. Such cases, involving Israel, Iran, Pakistan and Libya, have been analyzed in terms of international actors involved and methods deployed. Using international incident data contained in the Database on Nuclear Smuggling, Theft and Orphan Radiation Sources (DSTO) and international experience gained from the fight against drug trafficking, a generic Trafficking Pathway Model (TPM) is developed for trafficking of natural radionuclides. The TPM covers the complete trafficking cycle, ranging from material diversion, covert material transport, material concealment, and all associated operational procedures. The model subdivides the trafficking cycle into five phases: (1) Material diversion by insider(s) or initiation by outsider(s); (2) Covert transport; (3) Material brokerage; (4) Material sale; (5) Material delivery. An Action Plan is recommended, addressing the strengthening of the national infrastructure for material protection and accounting, development of higher standards of good governance, and needs for improving the control system deployed by customs, border guards and security forces.
NASA Astrophysics Data System (ADS)
Sims, D. J.
Soil samples have been taken in 2001 from the area of a 1951 release from an underground storage tank of 6.7 L of an aqueous solution of irradiated uranium (360 GBq). A simulation of the dispersion of the actinides and fission products was conducted in the laboratory using irradiated natural uranium, non-irradiated natural uranium and metal standards dissolved in acidic aqueous solutions and added to soil columns containing uncontaminated prairie soil. The lab soil columns were allowed 12 to 14 months for contaminant transport. Soil samples were analyzed using gamma-ray spectroscopy, neutron activation analysis (NAA) and liquid scintillation counting (LSC) to determine the elemental concentrations of U, Cs and Sr. Diffusion coefficients from the 50 year soil samples and the lab soil samples were determined. The measured diffusion coefficients from the field samples were 3.0 x 10-4 cm2 s-1 (Cs-137), 1.8 x 10-5 cm2 s-1 (U-238) and 2.6 x 10-3 cm2 s-1 (Sr-90) and the values determined from lab simulation were 5 x 10-6 cm 2 s-1 (Cs-137), 3 x 10-5 cm2 s-1 (U-238) and 1.9 x 10-5 cm 2 s-1 (Sr-90). The differences between the sets of diffusion coefficients can be attributed to differences in retardation effects, weather effects and changes in the soil characteristics when transporting, such as porosity. The analytical work showed that Cs-137 content of soil can be determined effectively using gamma-ray spectroscopy; U-238 content can be measured using NAA; and Sr-90 content can be measured using LSC. For non- and low-radioactive species, it was shown that both flame atomic absorption spectrometry (FAAS) and inductively-coupled plasma-mass spectrometry (ICP-MS) gave comparable results for Sr, Cs and Sm, with the average values ranging from 0.5 to 4.5 ppm of each other. The U-238 content results from NAA and from ICP-MS showed general agreement with an average difference of 81.3 ppm on samples having concentrations up to 988.2 ppm. The difference may have been due to matrix interference. It was determined through finite element modeling that 250 years after the 1951 release, the soil concentration of the three contaminant of U-238, Sr-90 and Cs-137 will be less than their respective soil clearance level values and therefore will not pose a long term environmental hazard. The fastest nuclide to reach the water table, at a depth of 45 m below the surface, at Suffield Site 27 was calculated to be Sr-90 after a period of 15,000 years. Therefore, it is not necessary to remove the subsurface soil at Site 27 for site decontamination but it is recommended that a "no-digging" policy, except for scientific research, be enforced at this site.
Li, W B; Karpas, Z; Salonen, L; Kurttio, P; Muikku, M; Wahl, W; Höllriegl, V; Hoeschen, C; Oeh, U
2009-06-01
To predict uranium in human hair due to chronic exposure through drinking water, a compartment representing human hair was added into the uranium biokinetic model developed by the International Commission on Radiological Protection (ICRP). The hair compartmental model was used to predict uranium excretion in human hair as a bioassay indicator due to elevated uranium intakes. Two excretion pathways, one starting from the compartment of plasma and the other from the compartment of intermediate turnover soft tissue, are assumed to transfer uranium to the compartment of hair. The transfer rate was determined from reported uranium contents in urine and in hair, taking into account the hair growth rate of 0.1 g d(-1). The fractional absorption in the gastrointestinal tract of 0.6% was found to fit best to describe the measured uranium levels among the users of drilled wells in Finland. The ingestion dose coefficient for (238)U, which includes its progeny of (234)Th, (234m)Pa, and (234)Pa, was calculated equal to 1.3 x 10(-8) Sv Bq(-1) according to the hair compartmental model. This estimate is smaller than the value of 4.5 x 10(-8) Sv Bq(-1) published by ICRP for the members of the public. In this new model, excretion of uranium through urine is better represented when excretion to the hair compartment is accounted for and hair analysis can provide a means for assessing the internal body burden of uranium. The model is applicable for chronic exposure as well as for an acute exposure incident. In the latter case, the hair sample can be collected and analyzed even several days after the incident, whereas urinalysis requires sample collection shortly after the exposure. The model developed in this study applies to ingestion intakes of uranium.
NASA Astrophysics Data System (ADS)
Kaur, Gurjit; Sandhu, Kirandeep; Kaur, Amandeep; Sharma, Manoj K.
2018-05-01
The dynamical cluster decay model is employed to investigate the decay of *265Db and *267Db nuclei, formed in the 27Al+238U , 18O+249Bk , and 19F+248Cm hot fusion reactions at energies around the Coulomb barrier. First, the fission dynamics of the 27Al+238U reaction is explored by investigating the fragmentation and preformation yield of the reaction. The symmetric mass distribution of the fission fragments is observed for *265Db nucleus, when static β2 i deformations are used within hot optimum orientation approach. However, the mass split gets broaden for the use of β2 i-dynamical hot configuration of the fragments and becomes clearly asymmetric for the cold-static-deformed approach. Within the application of cold orientations of fragments, a new fission channel is observed at mass asymmetry η =0.29 . In addition to 238U-induced reaction, the work is carried out to address the fission and neutron evaporation cross sections of *267Db nucleus formed via 19F+248Cm and 18O+249Bk reactions, besides a comprehensive analysis of fusion and capture processes. Higher fusion cross sections and compound nucleus formation probabilities (PCN) are obtained for the 18O+249Bk reaction, as larger mass asymmetry in the entrance channel leads to reduced Coulomb factor. Finally, the role of sticking (IS) and nonsticking (INS) moments of inertia is analyzed for the 4 n and 5 n channels of *267Db nuclear system.
Performance Evaluation of Spectroscopic Detectors for LEU Hold-up Measurements
DOE Office of Scientific and Technical Information (OSTI.GOV)
Venkataraman, Ramkumar; Nutter, Greg; McElroy, Robert Dennis
The hold-up measurement of low-enriched uranium materials may require use of alternate detector types relative to the measurement of highly enriched uranium. This is in part due to the difference in process scale (i.e., the components are generally larger for low-enriched uranium systems), but also because the characteristic gamma-ray lines from 235U used for assay of highly enriched uranium will be present at a much reduced intensity (on a per gram of uranium basis) at lower enrichments. Researchers at Oak Ridge National Laboratory examined the performance of several standard detector types, e.g., NaI(Tl), LaBr3(Ce), and HPGe, to select a suitablemore » candidate for measuring and quantifying low-enriched uranium hold-up in process pipes and equipment at the Portsmouth gaseous diffusion plant. Detector characteristics, such as energy resolution (full width at half maximum) and net peak count rates at gamma ray energies spanning a range of 60–1332 keV, were measured for the above-mentioned detector types using the same sources and in the same geometry. Uranium enrichment standards (Certified Reference Material no. 969 and Certified Reference Material no. 146) were measured using each of the detector candidates in the same geometry. The net count rates recorded by each detector at 186 keV and 1,001 keV were plotted as a function of enrichment (atom percentage). Background measurements were made in unshielded and shielded configurations under both ambient and elevated conditions of 238U activity. The highly enriched uranium hold-up measurement campaign at the Portsmouth plant was performed on process equipment that had been cleaned out. Therefore, in most cases, the thickness of the uranium deposits was less than the “infinite thickness” for the 186 keV gamma rays to be completely self-attenuated. Because of this, in addition to measuring the 186 keV gamma, the 1,001 keV gamma ray from 234mPa—a daughter of 238U in secular equilibrium with its parent—will also need to be measured. Based on the performance criteria of detection efficiency, energy resolution, peak-to-continuum ratios, minimum detectable limits, and the weight of the shielded probe, a shielded (0.5 in. thick lead shield) 2 × 2 in. NaI(Tl) detector is recommended for use. The recommended approach is to carry out analysis using data from both 186 keV and 1,001 keV gamma rays, and select a best result based on propagated uncertainty estimates. It is also highly recommended that a two-point gain stabilization scheme based on an 241Am seed embedded in the probe be implemented. Shielding configurations to reduce the impact of background interference on the measurement of 1,001 keV gamma-ray are discussed.« less
NASA Astrophysics Data System (ADS)
Metzger, Robert; Riper, Kenneth Van; Lasche, George
2017-09-01
A new method for analysis of uranium and radium in soils by gamma spectroscopy has been developed using VRF ("Visual RobFit") which, unlike traditional peak-search techniques, fits full-spectrum nuclide shapes with non-linear least-squares minimization of the chi-squared statistic. Gamma efficiency curves were developed for a 500 mL Marinelli beaker geometry as a function of soil density using MCNP. Collected spectra were then analyzed using the MCNP-generated efficiency curves and VRF to deconvolute the 90 keV peak complex of uranium and obtain 238U and 235U activities. 226Ra activity was determined either from the radon daughters if the equilibrium status is known, or directly from the deconvoluted 186 keV line. 228Ra values were determined from the 228Ac daughter activity. The method was validated by analysis of radium, thorium and uranium soil standards and by inter-comparison with other methods for radium in soils. The method allows for a rapid determination of whether a sample has been impacted by a man-made activity by comparison of the uranium and radium concentrations to those that would be expected from a natural equilibrium state.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Isselhardt, Brett H.
2011-09-01
Resonance Ionization Mass Spectrometry (RIMS) has been developed as a method to measure relative uranium isotope abundances. In this approach, RIMS is used as an element-selective ionization process to provide a distinction between uranium atoms and potential isobars without the aid of chemical purification and separation. We explore the laser parameters critical to the ionization process and their effects on the measured isotope ratio. Specifically, the use of broad bandwidth lasers with automated feedback control of wavelength was applied to the measurement of 235U/ 238U ratios to decrease laser-induced isotopic fractionation. By broadening the bandwidth of the first laser inmore » a 3-color, 3-photon ionization process from a bandwidth of 1.8 GHz to about 10 GHz, the variation in sequential relative isotope abundance measurements decreased from >10% to less than 0.5%. This procedure was demonstrated for the direct interrogation of uranium oxide targets with essentially no sample preparation. A rate equation model for predicting the relative ionization probability has been developed to study the effect of variation in laser parameters on the measured isotope ratio. This work demonstrates that RIMS can be used for the robust measurement of uranium isotope ratios.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moir, R.W.
1982-02-22
The fusion breeder is a fusion reactor designed with special blankets to maximize the transmutation by 14 MeV neutrons of uranium-238 to plutonium or thorium to uranium-233 for use as a fuel for fission reactors. Breeding fissile fuels has not been a goal of the US fusion energy program. This paper suggests it is time for a policy change to make the fusion breeder a goal of the US fusion program and the US nuclear energy program. The purpose of this paper is to suggest this policy change be made and tell why it should be made, and to outlinemore » specific research and development goals so that the fusion breeder will be developed in time to meet fissile fuel needs.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Moir, R.W.
1982-04-20
The fusion breeder is a fusion reactor designed with special blankets to maximize the transmutation by 14 MeV neutrons of uranium-238 to plutonium or thorium to uranium-233 for use as a fuel for fission reactors. Breeding fissile fuels has not been a goal of the US fusion energy program. This paper suggests it is time for a policy change to make the fusion breeder a goal of the US fusion program and the US nuclear energy program. The purpose of this paper is to suggest this policy change be made and tell why it should be made, and to outlinemore » specific research and development goals so that the fusion breeder will be developed in time to meet fissile fuel needs.« less
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.
Uranium oxide fuel cycle analysis in VVER-1000 with VISTA simulation code
NASA Astrophysics Data System (ADS)
Mirekhtiary, Seyedeh Fatemeh; Abbasi, Akbar
2018-02-01
The VVER-1000 Nuclear power plant generates about 20-25 tons of spent fuel per year. In this research, the fuel transmutation of Uranium Oxide (UOX) fuel was calculated by using of nuclear fuel cycle simulation system (VISTA) code. In this simulation, we evaluated the back end components fuel cycle. The back end component calculations are Spent Fuel (SF), Actinide Inventory (AI) and Fission Product (FP) radioisotopes. The SF, AI and FP values were obtained 23.792178 ton/y, 22.811139 ton/y, 0.981039 ton/y, respectively. The obtained value of spent fuel, major actinide, and minor actinide and fission products were 23.8 ton/year, 22.795 ton/year, 0.024 ton/year and 0.981 ton/year, respectively.
Modeling spallation reactions in tungsten and uranium targets with the Geant4 toolkit
NASA Astrophysics Data System (ADS)
Malyshkin, Yury; Pshenichnov, Igor; Mishustin, Igor; Greiner, Walter
2012-02-01
We study primary and secondary reactions induced by 600 MeV proton beams in monolithic cylindrical targets made of natural tungsten and uranium by using Monte Carlo simulations with the Geant4 toolkit [1-3]. Bertini intranuclear cascade model, Binary cascade model and IntraNuclear Cascade Liège (INCL) with ABLA model [4] were used as calculational options to describe nuclear reactions. Fission cross sections, neutron multiplicity and mass distributions of fragments for 238U fission induced by 25.6 and 62.9 MeV protons are calculated and compared to recent experimental data [5]. Time distributions of neutron leakage from the targets and heat depositions are calculated. This project is supported by Siemens Corporate Technology.
Whicker, Jeffrey J; Pinder, John E; Ibrahim, Shawki A; Stone, James M; Breshears, David D; Baker, Kristine N
2007-07-01
The environmental mobility of newly deposited radionuclides in surface soil is driven by complex biogeochemical relationships, which have significant impacts on transport pathways. The partition coefficient (Kd) is useful for characterizing the soil-solution exchange kinetics and is an important factor for predicting relative amounts of a radionuclide transported to groundwater compared to that remaining on soil surfaces and thus available for transport through erosion processes. Measurements of Kd for 238U are particularly useful because of the extensive use of 238U in military applications and associated testing, such as done at Los Alamos National Laboratory (LANL). Site-specific measurements of Kd for 238U are needed because Kd is highly dependent on local soil conditions and also on the fine soil fraction because 238U concentrates onto smaller soil particles, such as clays and soil organic material, which are most susceptible to wind erosion and contribute to inhalation exposure in off-site populations. We measured Kd for uranium in soils from two neighboring semiarid forest sites at LANL using a U.S. Environmental Protection Agency (EPA)-based protocol for both whole soil and the fine soil fraction (diameters<45 microm). The 7-d Kd values, which are those specified in the EPA protocol, ranged from 276-508 mL g-1 for whole soil and from 615-2249 mL g-1 for the fine soil fraction. Unexpectedly, the 30-d Kd values, measured to test for soil-solution exchange equilibrium, were more than two times the 7-d values. Rates of adsorption of 238U to soil from solution were derived using a 2-component (FAST and SLOW) exponential model. We found significant differences in Kd values among LANL sampling sites, between whole and fine soils, and between 7-d and 30-d Kd measurements. The significant variation in soil-solution exchange kinetics among the soils and soil sizes promotes the use of site-specific data for estimates of environmental transport rates and suggests possible differences in desorption rates from soil to solution (e.g., into groundwater or lung fluid). We also explore potential relationships between wind erosion, soil characteristics, and Kd values. Combined, our results highlight the need for a better mechanistic understanding of soil-solution partitioning kinetics for accurate risk assessment.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Denton, J. S.; Goldstein, S. J.; Paviet, P.
Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca inmore » the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Furthermore, uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface.« less
Meta-analysis of depleted uranium levels in the Middle East region.
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.
Separation of uranium isotopes by chemical exchange
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)
Hazardous Waste Surveys of Two Army Installations and an Army Hospital.
1980-08-01
232 Nickel-63 Uranium-238 Plutonium-239 Polonium - 210 6 Army Medical Treatment Facilities: General Administration Army Regulation (AR) 40-2, 42A peren...Categories 10 2 Waste Matrix 14 3 Search Format 16 4 Field Sanitation Unit Personal Health Supplies 19 5 Company Vehicle Maintenance Supplies...increasing industrialization of society, coupled with an equally increasing environmental and health safety awareness, has created a long list of wastes
Mirzadeh, S.; Lambrecht, R.M.
1985-07-01
The invention relates to a practical method for commercially producing radiopharmaceutical activities and, more particularly, relates to a method for the preparation of about equal amount of Radon-211 (/sup 211/Rn) and Xenon-125 (/sup 125/Xe) including a one-step chemical procedure following an irradiation procedure in which a selected target of Thorium (/sup 232/Th) or Uranium (/sup 238/U) is irradiated. The disclosed method is also effective for the preparation in a one-step chemical procedure of substantially equal amounts of high purity /sup 123/I and /sup 211/At. In one preferred arrangement of the invention almost equal quantities of /sup 211/Rn and /sup 125/Xe are prepared using a onestep chemical procedure in which a suitably irradiated fertile target material, such as thorium-232 or uranium-238, is treated to extract those radionuclides from it. In the same one-step chemical procedure about equal quantities of /sup 211/At and /sup 123/I are prepared and stored for subsequent use. In a modified arrangement of the method of the invention, it is practiced to separate and store about equal amounts of only /sup 211/Rn and /sup 125/Xe, while preventing the extraction or storage of the radionuclides /sup 211/At and /sup 123/I.
Kukreti, B M; Sharma, G K
2012-05-01
Accurate and speedy estimations of ppm range uranium and thorium in the geological and rock samples are most useful towards ongoing uranium investigations and identification of favorable radioactive zones in the exploration field areas. In this study with the existing 5 in. × 4 in. NaI(Tl) detector setup, prevailing background and time constraints, an enhanced geometrical setup has been worked out to improve the minimum detection limits for primordial radioelements K(40), U(238) and Th(232). This geometrical setup has been integrated with the newly introduced, digital signal processing based MCA system for the routine spectrometric analysis of low concentration rock samples. Stability performance, during the long counting hours, for digital signal processing MCA system and its predecessor NIM bin based MCA system has been monitored, using the concept of statistical process control. Monitored results, over a time span of few months, have been quantified in terms of spectrometer's parameters such as Compton striping constants and Channel sensitivities, used for evaluating primordial radio element concentrations (K(40), U(238) and Th(232)) in geological samples. Results indicate stable dMCA performance, with a tendency of higher relative variance, about mean, particularly for Compton stripping constants. Copyright © 2012 Elsevier Ltd. All rights reserved.
Detection Technology in the 21st Century: The Case of Nuclear Weapons of Mass Destruction
2008-03-26
Weapons of Mass Destruction FORMAT : Strategy Research Project DATE: 26 March 2008 WORD COUNT: 6,764 PAGES: 25 KEY TERMS: National Security, Deterrence...stocks remaining in Ukraine, Belarus, Uzbekistan, and other former Soviet and Eastern European states, and the unknown amounts of highly enriched uranium ...detect emissions from the decay of radioactive nuclides, which can occur naturally, such as uranium and thorium, or are manmade, such as plutonium
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.
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.
Defense Technical Information Center Thesaurus
2000-10-01
acquisition radar 4 + Indicates existence of further generic levels of the term DTIC Thesaurus Actuators Acridines Actinide series (cont.) Activated sintering...BT Heterocyclic compounds+ Uranium+ BT Sintering Acrilan Actinide series compounds Activated sludge process use Acrylonitrile polymers RT Actinide...Waste treatment+ Protactinium compounds Acronyms Thorium compounds+ Activation use Abbreviations Transuranium compounds+ UF Energizing Uranium compounds
NASA Astrophysics Data System (ADS)
White, A. M.; Ma, L.; Moravec, B. G.; McIntosh, J. C.; Chorover, J.
2017-12-01
In a remote, volcanic headwater catchment of the Jemez River Basin Critical Zone Observatory (JRB-CZO) in NM, stable water isotopes and solute chemistry have shown that snowmelt infiltrates and is stored before later discharging into springs and streams via subsurface flowpaths that vary seasonally. Therefore, water-rock reactions are also expected to change with season as hydrologic flowpaths transport water, gases and solutes through different biogeochemical conditions, rock types and fracture networks. Uranium-series isotopes have been shown to be a novel tracer of water-rock reactions and source water contributions while strontium isotopes are frequently used as indicators of chemical weathering and bedrock geology. This study combines both isotopes to understand how U and Sr isotope signatures evolve through the Critical Zone (CZ). More specifically, this work examines the relationship between seasonality, water transit time (WTT), and U-series and Sr isotopes in stream and spring waters from three catchments within the JRB-CZO, as well as lithology, rock type and CZ structure in solid phase cores. Samples from ten springs with known WTTs were analyzed for U and Sr isotopes to determine the effect of WTT on the isotopic composition of natural waters. Results suggest that WTT alone cannot explain the variability of U and Sr isotopes in JRB-CZO springs. Stream samples were also collected across two water years to establish how seasonality controls surface water isotopic composition. U and Sr isotope values vary with season, consistent with a previous study from the La Jara catchment; however, this study revealed that these changes do not show a systematic pattern among the three catchments suggesting that differences in the mineralogy and structure of the deep CZ in individual catchments, and partitioning of water along deep vs surficial and fracture vs matrix flow paths, likely also control isotopic variability. The distribution of U-series and Sr isotopes in core samples with depth shows distinct weathering profiles with variable 234U/238U activity and Sr isotope ratios. Comparison of the isotopic composition of cores and groundwaters from similar depths, as well as surface waters in the JRB-CZO will be vital for the characterization of hydrogeologic controls on isotopic composition in this complex terrain.
Electromagnetic fission of238U at 600 and 1000 MeV per nucleon
NASA Astrophysics Data System (ADS)
Rubehn, Th.; Müller, W. F. J.; Bassini, R.; Begemann-Blaich, M.; Blaich, Th.; Ferrero, A.; Groß, C.; Imme, G.; Iori, I.; Kunde, G. J.; Kunze, W. D.; Lindenstruth, V.; Lynen, U.; Möhlenkamp, T.; Moretto, L. G.; Ocker, B.; Pochodzalla, J.; Raciti, G.; Reito, S.; Sann, H.; Schüttauf, A.; Seidel, W.; Serfling, V.; Trautmann, W.; Trzcinski, A.; Verde, G.; Wörner, A.; Zude, E.; Zwieglinski, B.
1995-06-01
Electromagnetic fission of238U projectiles at E/A =600 and 1000 MeV was studied with the ALADIN spectrometer at the heavy-ion synchrotron SIS. Seven different targets (Be, C, Al, Cu, In, Au and U) were used. By considering only those fission events where the two charges added up to 92, most of the nuclear interactions were excluded. The nuclear contributions to the measured fission cross sections were determined by extrapolating from beryllium to the heavier targets with the concept of factorization. The obtained cross sections for electromagnetic fission are well reproduced by extended Weizsäcker-Williams calculations which include E1 and E2 excitations. The asymmetry of the fission fragments' charge distribution gives evidence for the excitation of the double giant-dipole resonance in uranium.
NASA Astrophysics Data System (ADS)
Bártová, H.; Kučera, J.; Musílek, L.; Trojek, T.; Gregorová, E.
2017-11-01
Knowledge of the content of natural radionuclides in bricks can be important in some cases in dosimetry and application of ionizing radiation. Dosimetry of naturally occurring radionuclides in matter (NORM) in general is one of them, the other one, related to radiation protection, is radon exposure evaluation, and finally, it is needed for the thermoluminescence (TL) dating method. The internal dose rate inside bricks is caused mostly by contributions of the natural radionuclides 238U, 232Th, radionuclides of their decay chains, and 40K. The decay chain of 235U is usually much less important. The concentrations of 238U, 232Th and 40K were measured by various methods, namely by gamma-ray spectrometry, X-ray fluorescence analysis (XRF), and neutron activation analysis (NAA) which was used as a reference method. These methods were compared from the point of view of accuracy, limit of detection (LOD), amount of sample needed and sample handling, time demands, and instrument availability.
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.
Accelerator Driven Nuclear Energy: The Thorium Option
Raja, Rajendran
2018-01-05
Conventional nuclear reactors use enriched Uranium as fuel and produce nuclear waste which needs to be stored away for over 10,000 years.  At the current rate of use, existing sources of Uranium will last for 50-100 years. We describe a solution to the problem that uses particle accelerators to produce fast neutrons that can be used to burn existing nuclear waste and produce energy. Such systems, initially proposed by Carlo Rubbia and collaborators in the 1990's, are being seriously considered by many countries as a possible solution to the green energy problem. Accelerator driven reactors operate in a sub-critical regime and, thus, are safer and can obtain energy from plentiful elements such as Thorium-232 and Uranium-238. What is missing is the high intensity (10MW) accelerator that produces 1 GeV protons. We will describe scenarios which if implemented will make such systems a reality. Â
DOE Office of Scientific and Technical Information (OSTI.GOV)
Havrilla, George Joseph; Gonzalez, Jhanis
2015-06-10
The use of femtosecond laser ablation inductively coupled plasma mass spectrometry was used to demonstrate the feasibility of measuring the isotopic ratio of uranium directly in U-10Mo fuel foils. The measurements were done on both the flat surface and cross sections of bare and Zr clad U-10Mo fuel foil samples. The results for the depleted uranium content measurements were less than 10% of the accepted U235/238 ratio of 0.0020. Sampling was demonstrated for line scans and elemental mapping over large areas. In addition to the U isotopic ratio measurement, the Zr thickness could be measured as well as trace elementalmore » composition if required. A number of interesting features were observed during the feasibility measurements which could provide the basis for further investigation using this methodology. The results demonstrate the feasibility of using fs-LA-ICP-MS for measuring the U isotopic ratio in U-10Mo fuel foils.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Donald, Scott B.; Siekhaus, Wigbert J.; Nelson, Art J.
X-ray photoelectron spectroscopy in combination with secondary ion mass spectrometry depth profiling were used to investigate the surface and interfacial chemistry of C + ion implanted polycrystalline uranium subsequently oxidized in air for over 10 years at ambient temperature. The original implantation of 33 keV C + ions into U 238 with a dose of 4.3 × 10 17 cm –3 produced a physically and chemically modified surface layer that was characterized and shown to initially prevent air oxidation and corrosion of the uranium after 1 year in air at ambient temperature. The aging of the surface and interfacial layersmore » were examined by using the chemical shift of the U 4f, C 1s, and O 1s photoelectron lines. In addition, valence band spectra were used to explore the electronic structure of the aged carbide surface and interface layer. Moreover, the time-of-flight secondary ion mass spectrometry depth profiling results for the aged sample confirmed an oxidized uranium carbide layer over the carbide layer/U metal interface.« less
Potential Aquifer Vulnerability in Regions Down-Gradient from ...
Sandstone-hosted roll-front uranium ore deposits originate when U(VI) dissolved in groundwater is reduced and precipitated as insoluble U(IV) minerals. Groundwater redox geochemistry, aqueous complexation, and solute migration are instrumental in leaching uranium from source rocks and transporting it in low concentrations to a chemical redox interface where it is deposited in an ore zone typically containing the uranium minerals uraninite, pitchblende, and/or coffinite; various iron sulfides; native selenium; clays; and calcite. In situ recovery (ISR) of these uranium ores is a process of contacting the uranium mineral deposit with leaching (lixiviant) fluids via injection of the lixiviant into wells drilled into the subsurface aquifer that hosts uranium ore, while other extraction wells pump the dissolved uranium after dissolution of the uranium minerals. Environmental concerns during and after ISR include water quality impacts from: 1) potential excursions of leaching solutions away from the injection zone into down-dip, underlying, or overlying aquifers; 2) potential migration of uranium and its decay products (e.g., Ra, Rn, Pb); and, 3) potential migration of redox-sensitive trace metals (e.g., Fe, Mn, Mo, Se, V), metalloids (e.g., As), and anions (e.g., sulfate). This review describes the geochemical processes that control roll-front uranium transport and fate in groundwater systems, identifies potential aquifer vulnerabilities to ISR operations, identifies
Natural radioactivity in stream sediments of Oltet River, Romania
NASA Astrophysics Data System (ADS)
Ion, Adriana
2017-04-01
The concentration of naturally occurring radionuclides (U-238, Th-232 and K-40) in stream sediments of the Oltet River was measured in order to establish the primary sources of radionuclides, the transport pathways and the geochemical factors favouring their mobilisation and concentration in the existing geological context. The Oltet River has a length of 185 Km and crosses the southern central part of the country, being the right tributary of the Olt River. The range in elevation of the watercourse varies between 1963 m in the springs area (Parîng Mountains) and 200 m at the confluence with the Olt River, whereas the relief of the Oltet Basin has a varied character, manifested by the presence of diverse forms of relief, starting with major mountainous heights and ending with low-lying plains regions. In cross section from North to South, the Olteț River cuts metamorphic rocks (schist, gneisses, quartzite, marble, mica-schist's), magmatic rocks (granite and granitoid massifs - intruded by veins of microgranite, aplite, pegmatite and lamprophyre) and limestone, followed by deposits composed of clays, marls, sands and gravels, that are characterized by the presence of lignite seams. 44 stream sediment samples were collected in summer of 2016 from sampling points distributed along the river with an equidistance of about 4 - 5 km. The activity concentrations of the U-238, Th-232 and K-40 were measured by gamma ray spectrometry using HPGe detector (ORTEC) with 26% relative efficiency in multilayer shielding. The reference materials used were IAEA - RGK-1 and IAEA - 314. Analysis was performed on the <2 mm fraction of sediment sample, each sample was counted for 24,000 s. U-238 specific activity in the stream sediments varies between 6.18 and 68.76 Bq/Kg and Th-232 specific activity from 8.12 to 89.28 Bq/Kg, whereas the K-40 specific activity in sediments ranges from 99.01 to 312.16 Bq/Kg. In the upper sector of the Oltet River, concentrations of U-238, Th-232 and K-40 show a good correlation between them and reflect the lithological features, the mechanical degradation of the rocks overcomes their chemical decomposition. In the middle part of the river as result of almost abrupt passage between mountain and hilly terrains increases and concentration of radionuclides; effect of large quantities of clastic material deposited by torrents. The mechanical migration of resistant uranium, thorium and potassium bearing mineral determines the movement of rock particles under moving water effect, and redistribution in alluvial sediments with preservation of the native features. In this zone under the action of biochemical processes and other chemical weathering agents, uranium is released from rocks and penetrates in the superficial circulation area or groundwater. Through this geochemical process the amounts of thorium and potassium released are modest, leaching of uranium being the dominant feature (uranyl ion). The downstream lignite seams are the secondary geochemical barriers in accumulation of uranium; the radiometric data obtained for stream sediments emphasize this enrichment.
Ages of subsurface stratigraphic intervals in the Quaternary of Enewetak Atoll, Marshall Islands
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.
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.
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.
The positron peak puzzle - Recent results from APEX
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
Kukreti, B M; Pandey, Pradeep; Singh, R V
2012-08-01
Non-coring based exploratory drilling was under taken in the sedimentary environment of Rangsohkham block, East Khasi Hills district to examine the eastern extension of existing uranium resources located at Domiasiat and Wakhyn in the Mahadek basin of Meghalaya (India). Although radiometric survey and radiometric analysis of surface grab/channel samples in the block indicate high uranium content but the gamma ray logging results of exploratory boreholes in the block, did not obtain the expected results. To understand this abrupt discontinuity between the two sets of data (surface and subsurface) multivariate statistical analysis of primordial radioactive elements (K(40), U(238) and Th(232)) was performed using the concept of representative subsurface samples, drawn from the randomly selected 11 boreholes of this block. The study was performed to a high confidence level (99%), and results are discussed for assessing the U and Th behavior in the block. Results not only confirm the continuation of three distinct geological formations in the area but also the uranium bearing potential in the Mahadek sandstone of the eastern part of Mahadek Basin. Copyright © 2012 Elsevier Ltd. All rights reserved.
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.
NASA Astrophysics Data System (ADS)
Panghal, Amanjeet; Kumar, Ajay; Kumar, Suneel; Singh, Joga; Sharma, Sumit; Singh, Parminder; Mehra, Rohit; Bajwa, B. S.
2017-06-01
Uranium gets into drinking water when the minerals containing uranium are dissolved in groundwater. Uranium and radon concentrations have been measured in drinking water samples from different water sources such as hand pumps, tube wells and bore wells at different depths from various locations of four districts (Jind, Rohtak, Panipat and Sonipat) of Haryana, India, using the LED flourimetry technique and RAD7, electronic silicon solid state detector. The uranium (238U) and radon (222Rn) concentrations in water samples have been found to vary from 1.07 to 40.25 µg L-1 with an average of 17.91 µg L-1 and 16.06 ± 0.97 to 57.35 ± 1.28 Bq L-1 with an average of 32.98 ± 2.45 Bq L-1, respectively. The observed value of radon concentration in 43 samples exceeded the recommended limits of 11 Bq L-1 (USEPA) and all the values are within the European Commission recommended limit of 100 Bq L-1. The average value of uranium concentration is observed to be within the safe limit recommended by World Health Organization (WHO) and Atomic Energy Regulatory Board. The annual effective dose has also been measured in all the water samples and is found to be below the prescribed dose limit of 100 µSv y-1 recommended by WHO. Risk assessment of uranium in water is also calculated using life time cancer risk, life time average daily dose and hazard quotient. The high uranium concentration observed in certain areas is due to interaction of ground water with the soil formation of this region and the local subsurface geology of the region.
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
Letter Report: Looking Ahead at Nuclear Fuel Resources
DOE Office of Scientific and Technical Information (OSTI.GOV)
J. Stephen Herring
2013-09-01
The future of nuclear energy and its ability to fulfill part of the world’s energy needs for centuries to come depend on a reliable input of nuclear fuel, either thorium or uranium. Obviously, the present nuclear fuel cycle is completely dependent on uranium. Future thorium cycles will also depend on 235U or fissile isotopes separated from used fuel to breed 232Th into fissile 233U. This letter report discusses several emerging areas of scientific understanding and technology development that will clarify and enable assured supplies of uranium and thorium well into the future. At the most fundamental level, the nuclear energymore » community needs to appreciate the origins of uranium and thorium and the processes of planetary accretion by which those materials have coalesced to form the earth and other planets. Secondly, the studies of geophysics and geochemistry are increasing understanding of the processes by which uranium and thorium are concentrated in various locations in the earth’s crust. Thirdly, the study of neutrinos and particularly geoneutrinos (neutrinos emitted by radioactive materials within the earth) has given an indication of the overall global inventories of uranium and thorium, though little indication for those materials’ locations. Crustal temperature measurements have also given hints of the vertical distribution of radioactive heat sources, primarily 238U and 232Th, within the continental crust. Finally, the evolving technologies for laser isotope separation are indicating methods for reducing the energy input to uranium enrichment but also for tailoring the isotopic vectors of fuels, burnable poisons and structural materials, thereby adding another tool for dealing with long-term waste management.« less
A theoretical study of alpha star populations in loaded nuclear emulsions
Senftle, F.E.; Farley, T.A.; Stieff, L.R.
1954-01-01
This theoretical study of the alpha star populations in loaded emulsions was undertaken in an effort to find a quantitative method for the analysis of less than microgram amounts of thorium in the presence of larger amounts of uranium. Analytical expressions for each type of star from each of the significantly contributing members of the uranium and thorium series as well as summation formulas for the whole series have been computed. The analysis for thorium may be made by determining the abundance of five-branched stars in a loaded nuclear emulsion and comparing of observed and predicted star populations. The comparison may also be used to check the half-lives of several members of the uranium and thorium series. ?? 1954.
LEACHING OF URANIUM ORES USING ALKALINE CARBONATES AND BICARBONATES AT ATMOSPHERIC PRESSURE
Thunaes, A.; Brown, E.A.; Rabbits, A.T.; Simard, R.; Herbst, H.J.
1961-07-18
A method of leaching uranium ores containing sulfides is described. The method consists of adding a leach solution containing alkaline carbonate and alkaline bicarbonate to the ore to form a slurry, passing the slurry through a series of agitators, passing an oxygen containing gas through the slurry in the last agitator in the series, passing the same gas enriched with carbon dioxide formed by the decomposition of bicarbonates in the slurry through the penultimate agitator and in the same manner passing the same gas increasingly enriched with carbon dioxide through the other agitators in the series. The conditions of agitation is such that the extraction of the uranium content will be substantially complete before the slurry reaches the last agitator.
Certified reference materials and reference methods for nuclear safeguards and security.
Jakopič, R; Sturm, M; Kraiem, M; Richter, S; Aregbe, Y
2013-11-01
Confidence in comparability and reliability of measurement results in nuclear material and environmental sample analysis are established via certified reference materials (CRMs), reference measurements, and inter-laboratory comparisons (ILCs). Increased needs for quality control tools in proliferation resistance, environmental sample analysis, development of measurement capabilities over the years and progress in modern analytical techniques are the main reasons for the development of new reference materials and reference methods for nuclear safeguards and security. The Institute for Reference Materials and Measurements (IRMM) prepares and certifices large quantities of the so-called "large-sized dried" (LSD) spikes for accurate measurement of the uranium and plutonium content in dissolved nuclear fuel solutions by isotope dilution mass spectrometry (IDMS) and also develops particle reference materials applied for the detection of nuclear signatures in environmental samples. IRMM is currently replacing some of its exhausted stocks of CRMs with new ones whose specifications are up-to-date and tailored for the demands of modern analytical techniques. Some of the existing materials will be re-measured to improve the uncertainties associated with their certified values, and to enable laboratories to reduce their combined measurement uncertainty. Safeguards involve the quantitative verification by independent measurements so that no nuclear material is diverted from its intended peaceful use. Safeguards authorities pay particular attention to plutonium and the uranium isotope (235)U, indicating the so-called 'enrichment', in nuclear material and in environmental samples. In addition to the verification of the major ratios, n((235)U)/n((238)U) and n((240)Pu)/n((239)Pu), the minor ratios of the less abundant uranium and plutonium isotopes contain valuable information about the origin and the 'history' of material used for commercial or possibly clandestine purposes, and have therefore reached high level of attention for safeguards authorities. Furthermore, IRMM initiated and coordinated the development of a Modified Total Evaporation (MTE) technique for accurate abundance ratio measurements of the "minor" isotope-amount ratios of uranium and plutonium in nuclear material and, in combination with a multi-dynamic measurement technique and filament carburization, in environmental samples. Currently IRMM is engaged in a study on the development of plutonium reference materials for "age dating", i.e. determination of the time elapsed since the last separation of plutonium from its daughter nuclides. The decay of a radioactive parent isotope and the build-up of a corresponding amount of daughter nuclide serve as chronometer to calculate the age of a nuclear material. There are no such certified reference materials available yet. Copyright © 2013 Elsevier Ltd. All rights reserved.
Extracting uranium from seawater: Promising AF series adsorbents
Das, Sadananda; Oyola, Y.; Mayes, Richard T.; ...
2015-11-02
Here, a new family of high surface area polyethylene fiber adsorbents (AF series) was recently developed at the Oak Ridge National Laboratory (ORNL). The AF series of were synthesized by radiation-induced graft polymerization of acrylonitrile and itaconic acid (at different monomer/co-monomer mol ratios) onto high surface area polyethylene fibers. The degree of grafting (%DOG) of AF series adsorbents was found to be 154 354%. The grafted nitrile groups were converted to amidoxime groups by treating with hydroxylamine. The amidoximated adsorbents were then conditioned with 0.44M KOH at 80 C followed by screening at ORNL with simulated seawater spiked with 8more » ppm uranium. Uranium adsorption capacity in simulated seawater screening ranged from 170-200 g-U/kg-ads irrespective of %DOG. A monomer/co-monomer mol ratio in the range of 7.57-10.14 seemed to be optimum for highest uranium loading capacity. Subsequently, the adsorbents were also tested with natural seawater at Pacific Northwest National Laboratory (PNNL) using flow-through exposure uptake experiments to determine uranium loading capacity with varying KOH conditioning time at 80 C. The highest adsorption capacity of AF1 measured after 56 days of marine testing was demonstrated as 3.9 g-U/kg-adsorbent and 3.2 g-U/kg-adsorbent for 1hr and 3hrs of KOH conditioning at 80 C, respectively. Based on capacity values of several AF1 samples, it was observed that changing KOH conditioning from 3hrs to 1hr at 80 C resulted in 22-27% increase in uranium loading capacity in seawater.« less
Extracting uranium from seawater: Promising AF series adsorbents
DOE Office of Scientific and Technical Information (OSTI.GOV)
Das, Sadananda; Oyola, Y.; Mayes, Richard T.
Here, a new family of high surface area polyethylene fiber adsorbents (AF series) was recently developed at the Oak Ridge National Laboratory (ORNL). The AF series of were synthesized by radiation-induced graft polymerization of acrylonitrile and itaconic acid (at different monomer/co-monomer mol ratios) onto high surface area polyethylene fibers. The degree of grafting (%DOG) of AF series adsorbents was found to be 154 354%. The grafted nitrile groups were converted to amidoxime groups by treating with hydroxylamine. The amidoximated adsorbents were then conditioned with 0.44M KOH at 80 C followed by screening at ORNL with simulated seawater spiked with 8more » ppm uranium. Uranium adsorption capacity in simulated seawater screening ranged from 170-200 g-U/kg-ads irrespective of %DOG. A monomer/co-monomer mol ratio in the range of 7.57-10.14 seemed to be optimum for highest uranium loading capacity. Subsequently, the adsorbents were also tested with natural seawater at Pacific Northwest National Laboratory (PNNL) using flow-through exposure uptake experiments to determine uranium loading capacity with varying KOH conditioning time at 80 C. The highest adsorption capacity of AF1 measured after 56 days of marine testing was demonstrated as 3.9 g-U/kg-adsorbent and 3.2 g-U/kg-adsorbent for 1hr and 3hrs of KOH conditioning at 80 C, respectively. Based on capacity values of several AF1 samples, it was observed that changing KOH conditioning from 3hrs to 1hr at 80 C resulted in 22-27% increase in uranium loading capacity in seawater.« less
ANALYSIS OF 2H-EVAPORATOR SCALE WALL [HTF-13-82] AND POT BOTTOM [HTF-13-77] SAMPLES
DOE Office of Scientific and Technical Information (OSTI.GOV)
Oji, L.
2013-06-21
Savannah River Remediation (SRR) is planning to remove a buildup of sodium aluminosilicate scale from the 2H-evaporator pot by loading and soaking the pot with heated 1.5 M nitric acid solution. Sampling and analysis of the scale material has been performed so that uranium and plutonium isotopic analysis can be input into a Nuclear Criticality Safety Assessment (NCSA) for scale removal by chemical cleaning. Historically, since the operation of the Defense Waste Processing Facility (DWPF), silicon in the DWPF recycle stream combines with aluminum in the typical tank farm supernate to form sodium aluminosilicate scale mineral deposits in the 2Hevaporatormore » pot and gravity drain line. The 2H-evaporator scale samples analyzed by Savannah River National Laboratory (SRNL) came from the bottom cone sections of the 2H-evaporator pot [Sample HTF-13-77] and the wall 2H-evaporator [sample HTF-13-82]. X-ray diffraction analysis (XRD) confirmed that both the 2H-evaporator pot scale and the wall samples consist of nitrated cancrinite (a crystalline sodium aluminosilicate solid) and clarkeite (a uranium oxy-hydroxide mineral). On “as received” basis, the bottom pot section scale sample contained an average of 2.59E+00 ± 1.40E-01 wt % total uranium with a U-235 enrichment of 6.12E-01 ± 1.48E-02 %, while the wall sample contained an average of 4.03E+00 ± 9.79E-01 wt % total uranium with a U-235 enrichment of 6.03E-01% ± 1.66E-02 wt %. The bottom pot section scale sample analyses results for Pu-238, Pu-239, and Pu-241 are 3.16E- 05 ± 5.40E-06 wt %, 3.28E-04 ± 1.45E-05 wt %, and <8.80E-07 wt %, respectively. The evaporator wall scale samples analysis values for Pu-238, Pu-239, and Pu-241 averages 3.74E-05 ± 6.01E-06 wt %, 4.38E-04 ± 5.08E-05 wt %, and <1.38E-06 wt %, respectively. The Pu-241 analyses results, as presented, are upper limit values. These results are provided so that SRR can calculate the equivalent uranium-235 concentrations for the NCSA. Results confirm that the uranium contained in the scale remains depleted with respect to natural uranium. SRNL did not calculate an equivalent U-235 enrichment, which takes into account other fissionable isotopes U-233, Pu-239 and Pu-241. The applicable method for calculation of equivalent U-235 will be determined in the NCSA.« less
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.
U, Pu, and Am nuclear signatures of the Thule hydrogen bomb debris.
Eriksson, Mats; Lindahl, Patric; Roos, Per; Dahlgaard, Henning; Holm, Elis
2008-07-01
This study concerns an arctic marine environment that was contaminated by actinide elements after a nuclear accident in 1968, the so-called Thule accident In this study we have analyzed five isolated hot particles as well as sediment samples containing particles from the weapon material for the determination of the nuclear fingerprint of the accident. We report that the fissile material in the hydrogen weapons involved in the Thule accident was a mixture of highly enriched uranium and weapon-grade plutonium and that the main fissile material was 235U (about 4 times more than the mass of 239Pu). In the five hot particles examined, the measured uranium atomic ratio was 235U/238U = 1.02 +/- 0.16 and the Pu-isotopic ratios were as follows: 24Pu/239Pu = 0.0551 +/- 0.0008 (atom ratio), 238Pu/239+240Pu = 0.0161 +/- 0.0005 (activity ratio), 241Pu/239+240Pu = 0.87 +/- 0.12 (activity ratio), and 241Am/ 239+240Pu = 0.169 +/- 0.005 (activity ratio) (reference date 2001-10-01). From the activity ratios of 241Pu/241Am, we estimated the time of production of this weapon material to be from the late 1950s to the early 1960s. The results from reanalyzed bulk sediment samples showed the presence of more than one Pu source involved in the accident, confirming earlier studies. The 238Pu/239+240PU activity ratio and the 240Pu/ 239Pu atomic ratio were divided into at least two Pu-isotopic ratio groups. For both Pu-isotopic ratios, one ratio group had identical ratios as the five hot particles described above and for the other groups the Pu isotopic ratios were lower (238Pu/ 239+240PU activity ratio approximately 0.01 and the 240Pu/P239Pu atomic ratio 0.03). On the studied particles we observed that the U/Pu ratio decreased as a function of the time these particles were present in the sediment. We hypothesis that the decrease in the ratio is due to a preferential leaching of U relative to Pu from the particle matrix.
Managing the Nuclear Fuel Cycle: Policy Implications of Expanding Global Access to Nuclear Power
2007-11-01
critical aspect of the nuclear fuel cycle for the United States, where longstanding nonproliferation policy discouraged commercial nuclear fuel...perhaps the most critical question in this decade for strengthening the nuclear nonproliferation regime: how can access to sensitive fuel cycle...process can take advantage of the slight difference in atomic mass between 235U and 238U. The typical enrichment process requires about 10 lbs of uranium
Superheavy nuclei from 48Ca-induced reactions
NASA Astrophysics Data System (ADS)
Oganessian, Yu. Ts.; Utyonkov, V. K.
2015-12-01
The discovery and investigation of the new region of superheavy nuclei at the DGFRS separator based on fusion reactions of 48Ca with 238U-249Cf target nuclei are reviewed. The production cross sections and summaries of the decay properties, including the results of the posterior experiments performed at the SHIP, BGS, and TASCA separators, as well as at the chemistry setups, are discussed and compared with the theoretical calculations and the systematic trends in the α-decay and spontaneous fission properties. The properties of the new nuclei, isotopes of elements 112-118, and their decay products demonstrate significant increases in the stability of the heaviest nuclei with increasing neutron number and closer approach to magic number N = 184.
Radioactivity of Fertilizer and China (NORM) in Japan
DOE Office of Scientific and Technical Information (OSTI.GOV)
Michikuni, Shimo; Yuka, Matsuura; Noriko, Itoh
2008-08-07
Radioactivity of 6 fertilizer samples, 7 china clay samples and 5 china glaze samples, which are commonly used in Japan, was measured using a NaI(Tl) scintillation spectrometer. Potassium activity of fertilizer was almost 540-740 Bq/kg, and the highest activity was 9,100 Bq/kg. Activity of fertilizer was 10 times higher for potassium than for uranium-series. Furthermore, these activities were 25 times for potassium and 18 times for uranium-series in comparison with those in natural soil. In china clay, activities of potassium, uranium-series nuclides and thorium-series nuclides were 543-823 Bq/kg, 74.6-94.3 Bq/kg, and 86.3-128 Bq/kg, respectively. These were 1.5-2.2, 2.1-2.6 and 2.3-3.5more » times higher than activity of common soil. Activity of glaze was almost equal to that of china clay.« less