Spatial and temporal variability of 234U/238U activity ratios in the Shu River,Central Asia

This study presents the temporal and spatial variability of ²³⁴U/²³⁸U activity ratios in the Shu River and provides interpretation to explain the downstream changes of uranium and the ²³⁴U/²³⁸U activity ratios in the study area. The positive linear correlation (R ² = 0.98, p < 0.001) between uranium concentration and specific electrical conductance is consistent with rock weathering and leaching as the major contributor of dissolved uranium in the studied area of the river. The ²³⁴U/²³⁸U activity ratio ranged between ~1.6 in the upper reaches of the river to ~1.15 furthest downstream. Activity ratios at specific sampling points do not show significant seasonal variability.     

A study of234U/238U ratios in groundwaters of Taiyuan area,Shanxi Province

Uranium contents and²³⁴U/²³⁸U ratios have been determined on 29 water samples from the Taiyuan area, Shanxi Province. The results show that the same artesian aquifer has similar uranium contents and²³⁴U/²³⁸U activity ratios, and the deeper aquifers have higher A. R. values but lower uranium contents. The A. R. values increase slightly towards groundwater flow in the artesian aquifers dominated by oxidizing ground waters. The Lancun Spring and the famous Jinci Spring belong to two different karst groundwater systems, i.e., the east and west karst groundwater systems. The recharge area of the Lancun Spring should cover the wide limestone outcrops of middle Ordovician in the northeast. The Ordovician fissure-karst ground water to the Jinci Spring is extensively mixed with fissure water in Carboniferous-Jurassic formations and seepage water from the Fenhe River.     

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

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.     

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

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

Use of 234U/238U disequilibrium in measuring chemical weathering rate of rocks

The rate of chemical weathering of rocks has been determined by using uranium as a natural isotopic tracer. The concentration of uranium and ²³⁴U/²³⁸U ratio in natural waters, rocks, and soils of the Preto river basin (Bahia State, Brazil) was measured by alpha-ray spectroscopy.The activity ratio U234/U238 measured in the various samples indicates the uranium fraction which is dissolved from rocks during the weathering process. The results obtained show that 1 m of rock needs 25,000 yr to be weathered in this region under present climatic conditions.     

Radioelements,radiogenic helium and age relationships for groundwaters from the granites at Stripa,Sweden

The solution of radioelements and radiogenic ⁴He by groundwaters in fractured rocks is dependent upon the radioelement distribution in the rock matrix and the extent of the rock-water interface. The ${}^{234}\text{U}{}^{238}\text{U}$ activity ratio and the dissolved U, Rn and He contents of such groundwaters respond to changes in the flow regime with time. Although ${}^{234}\text{U}{}^{238}\text{U}$ activity ratios change with groundwater residence time as a consequence of ²³⁴Th-recoil induced solution of ²³⁴U, the activity ratio is strongly influenced by the U distribution within fractures, by the extent of the rock-water interface and by the amount of ²³⁸U in solution. A model for the quantitative evaluation of these effects is presented.Groundwaters from depths up to 880 m in the Stripa granite have variable dissolved uranium contents and ${}^{234}\text{U}{}^{238}\text{U}$ activity ratios. The uranium geochemistry is primarily determined by variations in flow path rather than by groundwater age.Dissolved radiogenic ⁴He in the groundwaters increases with their depth of origin, and is dependent upon the U content of the granite and upon its fracture porosity. It increases with groundwater residence time but movement of ⁴He by diffusion and transport processes make the actual groundwater age indeterminate.     

Behavior of isotope (<Superscript>18</Superscript>O/<Superscript>16</Superscript>O, <Superscript>234</Superscript>U/<Superscript>238</Superscript>U) systems during the formation of uranium deposits of the “sandstone” type

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

Uranium isotopic disequilibrium for groundwater classification: first results on complexe terminal and continental intercalaire aquifers in Southern Tunisia

A fractionation of uranium (U) series into parent–daughter pairs – ²³⁴U and ²³⁸U – always occurs in natural waters, and the disequilibria between these is commonly used as a tracer of groundwater flow. We report here an interpretation of the U-content and U isotope disequilibria in groundwater sampled from the deep Complexe Terminal and Continental Intercalaire aquifers of southern Tunisia. Variations in both the contents of these isotopes (0.006–2.4 ppb) and ²³⁴U/²³⁸U activity ratios (ARs) (1.7–15.4) were observed. The data could be plotted in two distinct fields of reciprocal U concentration versus ²³⁴U/²³⁸U AR according to groundwater flow and regional bedrock differences. An initial assessment aimed at verifying whether the results of this investigation support those of previous hydrogeological and isotope studies, thereby suggesting that the disequilibrium between U isotopes in groundwater may represent a useful tool for hydrogeological investigations of deep and fossil groundwater. In addition, the disequilibrium can be used for quantifying the recharge or mixing rates between different formations with the aim of delineating the preferential outflow pattern or determining residence times of waters.     

Experimental evidence for U-U fractionation during granite weathering with implications for U/U in natural waters

The daughter to parent (²³⁴U/²³⁸U) activity ratio in natural waters is often out of secular radioactive equilibrium. The major reason for this disequilibrium is related to the energetic α-decay of ²³⁸U and differential release of ²³⁴U relative to ²³⁸U. This disequilibrium originates from (1) preferential release of more loosely bound ²³⁴U from damaged mineral lattice sites or; (2) direct recoil of ²³⁴Th into surrounding media from near mineral surface boundaries, however, it is unclear which of the two mechanisms is most important in nature. To better quantify the effects of preferential release of ²³⁴U, two continuous laboratory granite leaching experiments conducted over 1100 h were performed. The leachates were characterized by declining U concentrations with time and (²³⁴U/²³⁸U) initially greater than unity (up to 1.15), which changed to below unity during leaching (∼0.95). The early elevated (²³⁴U/²³⁸U) suggests that additional ²³⁴U is released into solution by preferential release of ²³⁴U from mineral phases. However, the excess ²³⁴U constitutes a finite pool of easy leachable ²³⁴U and the (²³⁴U/²³⁸U) values become lower than unity when this pool is used up. A model based on first-order kinetics, dissolution rates and preferential release of ²³⁴U from damaged lattice sites was developed and is able to quantitatively predict the observed pattern of (²³⁴U/²³⁸U) values and U concentrations for the two granite leaching experiments. Extending the modeling to longer time scales more comparable to natural systems shows that the production of waters with high (²³⁴U/²³⁸U) ratios can be achieved in two distinct regimes (1) slow weathering where the rate of directly recoiled ²³⁴U near mineral surfaces into waters is high; (2) fast weathering where the role of incipient chemical weathering and preferential release of loosely bound ²³⁴U are important. The model is able to explain apparent opposite correlations between physical erosion rates and (²³⁴U/²³⁸U) in waters and it provides a new framework that will be useful for examining weathering regimes, their timescales and their coupling with physical erosion.     

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

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 ${}^{238}\text{U}{}^{238}\text{U}$ 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 HCO₃^? 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 × 10¹⁰g/yr to the oceans, a value very similar to its removal rate from the oceans, 1.05 × 10¹⁰g/yr, estimated based on its correlation with HCO₃^? 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 ${}^{234}\text{U}{}^{238}\text{U}$ activity ratio of 1.20 ± 0.06ismissing. The residence time of uranium isotopes in the oceans estimated from the ²³⁸U concentration and the ${}^{234}\text{U}{}^{238}\text{U}$ 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/cm₂·10³ yr into the oceans (about 20% of its river supply) is necessitated.     

确定砂岩型铀矿矿化地段的铀、钍同位素证据

根据铀、钍同位素地球化学基本原理,对新疆伊梨盆地５１２矿床含矿砂岩的Ｕ、Ｔｈ含量及其＾２３４Ｕ／＾２３８Ｕ、＾２３０Ｔｈ／＾２３２Ｔｈ进行了测试,并在此基础上对含矿砂岩的氧化带、还原带和氧化还原过渡带特征进行了研究。研究表明,与氧化带、还原带相比,氧化－还原过渡带具有较高Ｕ含量和＾２３４Ｕ／＾２３８Ｕ比值,较低Ｔｈ／Ｕ比值;矿石样品中的＾２３４Ｕ／＾２３８Ｕ、＾２３０Ｔｈ／＾２３８Ｕ比值位于过渡带     

State of disequilibrium between 238U, 234U, 226Ra and 222Rn in groundwater from bedrock

Approximately one thousand drilled wells were investigated for their natural radioactivity. The determinations of ²³⁸U, ²³⁴U, ²²⁶Ra and ²²²Rn from 310 samples showed a high state of radioactive disequilibrium between the members of the uranium series present in water. The ${}^{238}\text{U}{}^{226}\text{Ra}$ activity ratio usually fell in the range 1–20 and the ${}^{238}\text{U}{}^{222}\text{Rn}$ activity ratio in the range 1–20 × 10^?4, the highest activity ratios being from samples with an elevated uranium content. The ${}^{234}\text{U}{}^{238}\text{U}$ activity ratio varied between 0.76 and 4.67, the most frequent values showing a 60% excess of ²³⁴U in the samples. Most of the ${}^{234}\text{U}{}^{238}\text{U}$ activity ratios near unity were found in samples with a high uranium content. Several drilled wells with anomalously high uranium contents were found in southern Finland. The average ²²⁶Ra and ²²²Rn contents of these wells were not exceptionally high, which suggests high mobility of uranium in groundwater from the areas involved.     

Uranium series dating of stalagmites from Blanchard Springs Caverns,U.S.A.

Because stalagmites are enriched in ²³⁴U beyond the equilibrium value at the time of deposition, they are potentially datable by measuring their progress toward equilibrium. Procedures for uranium-thorium and uranium disequilibrium dating of speleothems were developed, making use of alpha spectrometry for thorium determinations and mass spectrometry for uranium determinations. The stalagmites tested were generally beyond the age range of the U-Th age dating method and, as a result, ²³⁴U/²³⁸U ratios provided the most useful dating technique. The estimated age range for a stalagmite from Blanchard Springs is 135,000 to 785,000 years BP with an interval of slow or suspended growth from about 320,000 to 570,000 years BP.     

Uranium isotopes as a tracer of sources of dissolved solutes in the Han River,South Korea

The uranium (U) content and ²³⁴U/²³⁸U activity ratio were determined for water samples collected from Korea's Han River in spring, summer, and winter 2006 to provide data that might constrain the origin of U isotope fractionation in river water and the link between U isotope systematics in river waters and the lithological nature of the corresponding bedrock. The large difference in the major dissolved loads between the two major branches of the Han River, the North Han River (NHR) and South Han River (SHR), is reflected in the contrasting U content and ²³⁴U/²³⁸U activity ratio between the tributaries: low U content (0.08–0.75 nM; average, 0.34 nM) and small ²³⁴U/²³⁸U activity ratio (1.03–1.22; average, 1.09) in the NHR; and high U content (0.65–1.98 nM; average, 1.44 nM) and large ²³⁴U/²³⁸U activity ratio (1.05–1.45; average, 1.24) in the SHR. The large spatial differences in U content and ²³⁴U/²³⁸U activity ratio are closely related to both lithological differences between the two tributaries and groundwater input. The low U content and small ²³⁴U/²³⁸U activity ratio in the NHR arise mainly from a combination of surface and meteoric weathering of the dominant silicate rocks in this branch and congruent dissolution of already weathered (secular equilibrium) materials. In contrast, the high U content and large ²³⁴U/²³⁸U activity ratio in the SHR are ascribed to the dissolution of carbonates and black shales along with significant inputs of deep groundwater.     

Uranium series disequilibria in the sedimentary uranium deposit at Yeelirrie,Western Australia

The weighted mean values of the ²³⁴U/²³⁸U and the ²³⁰Th/²³⁴U ratios in ore samples collected above the modern water table of the Yeelirrie uranium deposit in Western Australia are 1.38 ± 0.10 and 0.83 ± 0.28, respectively. The relatively larger variability in the latter ratio is evidence for the translocation of uranium subsequent to deposition. Daughter product separation is due to differences in the mobilities of the thorium and uranium species. Factors involved in interpreting the observed ratios, in terms of the dynamics of the accumulation of the deposit, are assessed in terms of an open system model. The observed disequilibria provide a quantitative basis for the evaluation of hypotheses developed from geological and other considerations.     

Fixation of radionuclides in the 238U decay series in the vicinity of mineralized zones: 1. The Austatom Uranium Prospect,Northern Territory,Australia

The minimum age of a zone of secondary uranium mineralization, located at the Austatom Prospect in the Alligator Rivers region of Australia, is estimated to be 3.6 × 10⁵y. This is derived from a geochronological model based on retarded leaching of ²³⁴U with respect to ²³⁸U and on ratios within the ore of these members of the ²³⁸U decay series. Although kaolinite is a dominant mineral in the weathered schist-host-rocks, retarded dissolution of ²³⁴U occurs only in the presence of the clay minerals illite and montmorillonite. In their absence the reverse occurs. A model is proposed to explain the results. Ratios of ²³⁰Th to ²³⁸U indicate that the mineralization has probably remained stationary within the weathered schist for at least 1 to 2 × 10⁵y. Future use of clay minerals as buffers in radioactive waste repositories is supported by the excellent long-term retention obtained for oxidized uranium, probably due in part to isomorphic substitution into the clay crystal lattice.     

Geo-chemical Behavior of Uranium in the Sambhar Salt Lake, Rajasthan (India): Implications to "Source" of Salt and Uranium "Sink"

Among several salt lakes in the Thar Desert of western India, the Sambhar is the largest lake producing about 2 × 10⁵ tons of salt (NaCl) annually. The “lake system” (lake waters, inflowing river waters, and sub-surface brines) provides a unique setting to study the geo-chemical behavior of uranium isotopes (²³⁸U, ²³⁴U) in conjunction with the evolution of brines over the annual wetting and evaporation cycles. The concentration of ²³⁸U and the total dissolved solids (TDS) in lake water increase from ~8 μg L⁻¹ and ~8 g L⁻¹ in monsoon to ~1,400 μg L⁻¹ and 370 g L⁻¹, respectively, during summer time. The U/TDS ratio (~1 μg g⁻¹ salt) and the ²³⁴U/²³⁸U activity ratio (1.65 ± 0.05), however, remain almost unchanged throughout the year, except when U/TDS ratio approaches to 3.8 at/or beyond halite crystallization. These observations suggest that uranium behaves conservatively in the lake waters during the annual cycle of evaporation. Also, uranium and salt content (TDS) are intimately coupled, which has been used to infer the origin and source of salt in the lake basin. Furthermore, near uniform ratios in evaporating lake waters, when compared to the ratio in seawater (~0.1 μg g⁻¹ salt and 1.14 ± 0.02, respectively), imply that aeolian transport of marine salts is unlikely to be significant source of salt to the lake in the present-day hydrologic conditions. This inference is further consistent with the chemical composition of wet-precipitation occurring in and around the Sambhar lake. The seasonal streams feeding the lake and groundwaters (within the lake’s periphery) have distinctly different ratios of U/TDS (2–69 μg g⁻¹ salt) and ²³⁴U/²³⁸U (1.15–2.26) compared to those in the lake. The average U/TDS ratio of ~1 μg g⁻¹ salt in lake waters and ~19 μg g⁻¹ salt in river waters suggest dilution of the uranium content by the recycled salt and/or removal processes presently operating in the lake during the extraction of salt for commercial use. Based on mass-balance calculations, a conservative estimate of "uranium sink" (in the form of bittern crust) accounts for ~5 tons year⁻¹ from the lake basin, an estimate similar to its input flux from rivers, i.e., 4.4 tons year⁻¹.     

A method for determination of the isotopic composition of authigenic uranium in Baikal bottom sediments

A simple, reliable, and high-performance method has been proposed for direct determination of the isotopic composition of authigenic uranium in silica lacustrine sediments. The method is based on studying the kinetics of the selective extraction of authigenic uranium from sediments with weak solutions of ammonium hydrocarbonate followed by the ICP-MS analysis of the nuclides. To estimate the contamination of authigenic uranium by terrigenous one, the contents of ²³²Th and some other clastogenic elements in the extracts were measured simultaneously. The selectivity of extraction of authigenic uranium from the sediments treated with a 1% NH₄HCO₃ solution appeared to be no worse than 99%. The method was used to analyze the isotopic composition of authigenic uranium at several key horizons of a core dated before. The measurements directly prove that the ²³⁴U/²³⁸U values in Baikal water varied depending on climate, which contradicts the previous statements. The measured ²³⁴U/²³⁸U ratios in paleo-Baikal water match the values reconstructed from isotopic data for total uranium in the sediments on the supposition that the U/Th ratio is constant in the terrigenous part of the sediment. Direct experimental determination of total and authigenic nuclides in sediments enhances the potentiality of the method for absolute ²³⁴U-²³⁰Th dating of carbonate-barren lacustrine sediments, including those from Lake Baikal, within the intervals corresponding to the periods of glaciation, where the sediments contain a large fraction of terrigenous component. Given the fractions of terrigenous and authigenic uranium are accurately determined, we have an opportunity to study the variability of the sources of terrigenous matter and to refine the previous model for reconstructing the climate humidity in East Siberia.     

U-series isotopic composition of kasolite associated with aplite-pegmatite at Jabal Sayid,Hijaz region,Kingdom of Saudi Arabia

Uranium and thorium isotopic composition of kasolite [Pb(UO₂)SiO₄-(H₂O)] from Jabal Sayid area was determined by thermal ionization mass spectrometry. Secondary electron imaging, back-scattered electron imaging, and energy dispersive spectral scans were used to investigate the mineralogical characteristics of this uranyl mineral phase. Distinct crystal faces and crystal growth of kasolite from the study area confirm mineral precipitation near the surface from the circulating groundwater. The obtained data were used to interpret the mechanism of uranium mobility in Jabal Sayid weathering profile and to construct a tentative model to explain the isotopic evolution of uranium and thorium. This model indicates that (1) uranium was leached at depth, (2) uranyl mineralization was precipitated along fractures and cavities in the host rocks during humid conditions and pluvial periods, (3) preferential leaching of ²³⁴U from uranyl mineralization by recoil processes was continuous indicative of a weakly circulating groundwater, and (4) ²³⁴U-deficiency resulted in isotopic signatures characterized by low ²³⁴U/²³⁸U and high ²³⁰Th/²³⁴U ratios. The modification pattern of these activity ratios suggests that uranyl mineralization of Jabal Sayid, most probably, has been precipitated during the same Late Quaternary pluvial periods responsible for the formation of the corresponding mineralizations in the Eastern Desert of Egypt.     

Weathering rates at Alto Sorocaba basin,Brazil, using U-isotopes and major cations

The aim of this paper was to evaluate the chemical weathering rate at Alto Sorocaba basin, São Paulo State, Brazil, as it is an important parameter on geomorphological characterization of continents. Several tools may be used for such evaluation, and this work compares the results obtained from analytical data involving the uranium concentration, the ²³⁴U/²³⁸U activity ratio and the major cation concentration for samples of waters, soils, and rocks from that basin. The use of the natural uranium as a tracer in weathering rate rocks studies is advantageous since this element is virtually absent in rainwater and also allows obtaining the dissolution rocks coefficient by the ²³⁴U/²³⁸U activity ratio. The Alto Sorocaba basin has serious environmental problems in terms of the quality of the rainwater and river waters, and, consequently, the geochemical balance using the main cations presented some difficulties. However, measuring of the weathering rate utilizing the U-isotopes method corresponded to 14 μm/year that allows estimating a time of 72,000 years to weather 1 m of rock at Sorocaba River upstream from Itupararanga Reservoir, under the present climatic conditions.