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1.
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.  相似文献   

2.
Calcite-rich soils (calcrete) in alluvium and colluvium at Solitario Wash, Crater Flat, Nevada, USA, contain pedogenic calcite and opaline silica similar to soils present elsewhere in the semi-arid southwestern United States. Nevertheless, a ground-water discharge origin for the Solitario Wash soil deposits was proposed in a series of publications proposing elevation-dependent variations of carbon and oxygen isotopes in calcrete samples. Discharge of ground water in the past would raise the possibility of future flooding in the unsaturated zone at Yucca Mountain, Nevada, site of a proposed high-level nuclear waste repository. New geochemical and carbon, oxygen, strontium, and uranium-series isotopic data disprove the presence of systematic elevation-isotopic composition relations, which are the main justification given for a proposed ground-water discharge origin of the calcrete deposits at Solitario Wash. Values of δ13C (−4.1 to −7.8 per mil [‰]), δ18O (23.8–17.2‰), 87Sr/86Sr (0.71270–0.71146), and initial 234U/238U activity ratios of about 1.6 in the new calcrete samples are within ranges previously observed in pedogenic carbonate deposits at Yucca Mountain and are incompatible with a ground-water origin for the calcrete. Variations in carbon and oxygen isotopes in Solitario Wash calcrete likely are caused by pedogenic deposition from meteoric water under varying Quaternary climatic conditions over hundreds of thousands of years.  相似文献   

3.
The goal of this study is to explain the origin of 234U–238U fractionation in groundwater from sedimentary aquifers of the St. Lawrence Lowlands (Quebec, Canada), and its relationship with 3He/4He ratios, to gain insight regarding the evolution of groundwater in the region. (234U/238U) activity ratios, or (234U/238U)act, were measured in 23 groundwater samples from shallow Quaternary unconsolidated sediments and from the deeper fractured regional aquifer of the Becancour River watershed. The lowest (234U/238U)act, 1.14 ± 0.01, was measured in Ca–HCO3-type freshwater from the Quaternary Shallower Aquifer, where bulk dissolution of the carbonate allows U to migrate into water with little 234U–238U isotopic fractionation. The (234U/238U)act increases to 6.07 ± 0.14 in Na–HCO3–Cl-type groundwater. Preferential migration of 234U into water by α-recoil is the underlying process responsible for this isotopic fractionation. An inverse relationship between (234U/238U)act and 3He/4He ratios has been observed. This relationship reflects the mixing of newly recharged water, with (234U/238U)act close to the secular equilibrium and containing atmospheric/tritiogenic helium, and mildly-mineralized older water (14C ages of 6.6 kyrs), with (234U/238U)act of ≥6.07 and large amounts of radiogenic 4He, in excess of the steady-state amount produced in situ. The simultaneous fractionation of (234U/238U)act and the addition of excess 4He could be locally controlled by stress-induced rock fracturing. This process increases the surface area of the aquifer matrix exposed to pore water, from which produced 4He and 234U can be released by α-recoil and diffusion. This process would also facilitate the release of radiogenic helium at rates greater than those supported by steady-state U–Th production in the rock. Consequently, sources internal to the aquifers could cause the radiogenic 4He excesses measured in groundwater.  相似文献   

4.
《Applied Geochemistry》2002,17(6):659-682
This paper provides a geologic and hydrologic framework of the Yucca Mountain region for the geochemical papers in this volume. The regional geologic units, which range in age from late Precambrian through Holocene, are briefly described. Yucca Mountain is composed of dominantly pyroclastic units that range in age from 11.4 to 15.2 Ma. The principal focus of study has been on the Paintbrush Group, which includes two major zoned and welded ash-flow tuffs separated by an important hydrogeologic unit referred to as the Paintbrush non-welded (PTn). The regional structural setting is currently one of extension, and the major local tectonic domains are presented together with a tectonic model that is consistent with the known structures at Yucca Mountain. Streamflow in this arid to semi-arid region occurs principally in intermittent or ephemeral channels. Near Yucca Mountain, the channels of Fortymile Wash and Amargosa River collect infrequent runoff from tributary basins, ultimately draining to Death Valley. Beneath the surface, large-scale interbasin flow of groundwater from one valley to another occurs commonly in the region. Regional groundwater flow beneath Yucca Mountain originates in the high mesas to the north and returns to the surface either in southern Amargosa Desert or in Death Valley, where it is consumed by evapotranspiration. The water table is very deep beneath the upland areas such as Yucca Mountain, where it is 500–750 m below the land surface, providing a large thickness of unsaturated rocks that are potentially suitable to host a nuclear-waste repository. The nature of unsaturated flow processes, which are important for assessing radionuclide migration, are inferred mainly from hydrochemical or isotopic evidence, from pneumatic tests of the fracture systems, and from the results of in situ experiments. Water seeping down through the unsaturated zone flows rapidly through fractures and more slowly through the pores of the rock matrix. Although capillary forces are expected to divert much of the flow around repository openings, some may drip onto waste packages, ultimately causing release of radionuclides, followed by transport down to the water table.  相似文献   

5.
Bulk dissolution rates for sediment from ODP Site 984A in the North Atlantic are determined using the 234U/238U activity ratios of pore water, bulk sediment, and leachates. Site 984A is one of only several sites where closely spaced pore water samples were obtained from the upper 60 meters of the core; the sedimentation rate is high (11-15 cm/ka), hence the sediments in the upper 60 meters are less than 500 ka old. The sediment is clayey silt and composed mostly of detritus derived from Iceland with a significant component of biogenic carbonate (up to 30%).The pore water 234U/238U activity ratios are higher than seawater values, in the range of 1.2 to 1.6, while the bulk sediment 234U/238U activity ratios are close to 1.0. The 234U/238U of the pore water reflects a balance between the mineral dissolution rate and the supply rate of excess 234U to the pore fluid by α-recoil injection of 234Th. The fraction of 238U decays that result in α-recoil injection of 234U to pore fluid is estimated to be 0.10 to 0.20 based on the 234U/238U of insoluble residue fractions. The calculated bulk dissolution rates, in units of g/g/yr are in the range of 4 × 10−7 to 2 × 10−6 yr−1. There is significant down-hole variability in pore water 234U/238U activity ratios (and hence dissolution rates) on a scale of ca. 10 m. The inferred bulk dissolution rate constants are 100 to 104 times slower than laboratory-determined rates, 100 times faster than rates inferred for older sediments based on Sr isotopes, and similar to weathering rates determined for terrestrial soils of similar age. The results of this study suggest that U isotopes can be used to measure in situ dissolution rates in fine-grained clastic materials.The rate estimates for sediments from ODP Site 984 confirm the strong dependence of reactivity on the age of the solid material: the bulk dissolution rate (Rd) of soils and deep-sea sediments can be approximately described by the expression Rd ≈ 0.1 Age−1 for ages spanning 1000 to 5 × 108 yr. The age of the material, which encompasses the grain size, surface area, and other chemical factors that contribute to the rate of dissolution, appears to be a much stronger determinant of dissolution rate than any single physical or chemical property of the system.  相似文献   

6.
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.  相似文献   

7.
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.  相似文献   

8.
《Applied Geochemistry》2002,17(6):709-734
Uranium, Th and Pb isotopes were analyzed in layers of opal and chalcedony from individual mm- to cm-thick calcite and silica coatings at Yucca Mountain, Nevada, USA, a site that is being evaluated for a potential high-level nuclear waste repository. These calcite and silica coatings on fractures and in lithophysal cavities in Miocene-age tuffs in the unsaturated zone (UZ) precipitated from descending water and record a long history of percolation through the UZ. Opal and chalcedony have high concentrations of U (10 to 780 ppm) and low concentrations of common Pb as indicated by large values of 206Pb/204Pb (up to 53,806), thus making them suitable for U-Pb age determinations. Interpretations of U-Pb isotope systems in opal samples at Yucca Mountain are complicated by the incorporation of excess 234U at the time of mineral formation, resulting in reverse discordance of U-Pb ages. However, the 207Pb/235U ages are much less affected by deviation from initial secular equilibrium and provide reliable ages of most silica deposits between 0.6 and 9.8 Ma. For chalcedony subsamples showing normal age discordance, these ages may represent minimum times of deposition. Typically, 207Pb/235U ages are consistent with the microstratigraphy in the mineral coating samples, such that the youngest ages are for subsamples from outer layers, intermediate ages are from inner layers, and oldest ages are from innermost layers. 234U and 230Th in most silica layers deeper in the coatings are in secular equilibrium with 238U, which is consistent with their old age and closed system behavior during the past ∼0.5 Ma. The ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from lithophysal cavities in the welded part of the Topopah Spring Tuff yield slow long-term average growth rates of 1 to 5 mm/Ma. These data imply that the deeper parts of the UZ at Yucca Mountain maintained long-term hydrologic stability over the past 10 Ma. despite significant climate variations. U-Pb ages for subsamples of silica layers from different microstratigraphic positions in individual calcite and silica coating samples collected from fractures in the shallower part of the UZ (welded part of the overlying Tiva Canyon Tuff) indicate larger long-term average growth rates up to 23 mm/Ma and an absence of recently deposited materials (ages of outermost layers are 3–5 Ma.). These differences between the characteristics of the coatings for samples from the shallower and deeper parts of the UZ may indicate that the nonwelded tuffs (PTn), located between the welded parts of the Tiva Canyon and Topopah Spring Tuffs, play an important role in moderating UZ flow.  相似文献   

9.
Uranium (U) concentrations and activity ratios (δ234U) of authigenic carbonates are sensitive recorders of different fluid compositions at submarine seeps of hydrocarbon-rich fluids (“cold seeps”) at Hydrate Ridge, off the coast of Oregon, USA. The low U concentrations (mean: 1.3 ± 0.4 μg/g) and high δ234U values (165-317‰) of gas hydrate carbonates reflect the influence of sedimentary pore water indicating that these carbonates were formed under reducing conditions below or at the seafloor. Their 230Th/234U ages span a time interval from 0.8 to 6.4 ka and cluster around 1.2 and 4.7 ka. In contrast, chemoherm carbonates precipitate from marine bottom water marked by relatively high U concentrations (mean: 5.2 ± 0.8 μg/g) and a mean δ234U ratio of 166 ± 3‰. Their U isotopes reflect the δ234U ratios of the bottom water being enriched in 234U relative to normal seawater. Simple mass balance calculations based on U concentrations and their corresponding δ234U ratios reveal a contribution of about 11% of sedimentary pore water to the bottom water. From the U pore water flux and the reconstructed U pore water concentration a mean flow rate of about 147 ± 68 cm/a can be estimated. 230Th/234U ages of chemoherm carbonates range from 7.3 to 267.6 ka. 230Th/234U ages of two chemoherms (Alvin and SE-Knoll chemoherm) correspond to time intervals of low sealevel stands in marine isotope stages (MIS) 2, 4, 5, 6, 7 and 8. This observation indicates that fluid flow at cold seep sites sensitively reflects pressure changes of the hydraulic head in the sediments. The δ18OPDB ratios of the chemoherm carbonates support the hypothesis of precipitation during glacial times. Deviations of the chemoherm δ18O values from the marine δ18O record can be interpreted as to reflect temporally and spatially varying bottom water and/or vent fluid temperatures during carbonate precipitation between 2.6 and 8.6°C.  相似文献   

10.
Both chemical weathering rates and fluid flow are difficult to measure in natural systems. However, these parameters are critical for understanding the hydrochemical evolution of aquifers, predicting the fate and transport of contaminants, and for water resources/water quality considerations. 87Sr/86Sr and (234U/238U) activity ratios are sensitive indicators of water-rock interaction, and thus provide a means of quantifying both flow and reactivity. The 87Sr/86Sr values in ground waters are controlled by the ratio of the dissolution rate to the flow rate. Similarly, the (234U/238U) ratio of natural ground waters is a balance between the flow rate and the dissolution of solids, and α-recoil loss of 234U from the solids. By coupling these two isotope systems it is possible to constrain both the long-term (ca. 100’s to 1000’s of years) flow rate and bulk dissolution rate along the flow path. Previous estimates of the ratio of the dissolution rate to the infiltration flux from Sr isotopes (87Sr/86Sr) are combined with a model for (234U/238U) to constrain the infiltration flux and dissolution rate for a 70-m deep vadose zone core from Hanford, Washington. The coupled model for both (234U/238U) ratios and the 87Sr/86Sr data suggests an infiltration flux of 5 ± 2 mm/yr, and bulk silicate dissolution rates between 10−15.7 and 10−16.5 mol/m2/s. The process of α-recoil enrichment, while primarily responsible for the observed variation in (234U/238U) of natural systems, is difficult to quantify. However, the rate of this process in natural systems affects the interpretation of most U-series data. Models for quantifying the α-recoil loss fraction based on geometric predictions, surface area constraints, and chemical methods are also presented. The agreement between the chemical and theoretical methods, such as direct measurement of (234U/238U) of the small grain size fraction and geometric calculations for that size fraction, is quite good.  相似文献   

11.
《Applied Geochemistry》2002,17(6):781-792
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.  相似文献   

12.
A mathematical model to calculate the234U/238U activity ratio (AR) in an aqueous phase in contact with rock/soil is presented. The model relies on the supply of238U by dissolution and that of234U by dissolution and preferential release from radiation damaged regions (recoil tracks). The model predicts that values of234U/238U AR>1 in the aqueous phase can be obtained only from weathering “virgin” surfaces. Thus, to account for the observed steady-state supply of234U excess to the oceans by the preferential leaching model, ‘virgin’ rock/soil surfaces would have to be continually exposed and weathered. The238U concentration and234U/238U AR in continental waters allow us to estimate the exposure rates of “virgin” rock/soil surfaces.  相似文献   

13.
Dissolved U concentrations and activity ratios (ARs) of the U isotopes in the 238U decay series were measured in ground and surface waters as part of an investigation to delineate the water quality in a proposed uranium mining area of northwest Nebraska. In oxidizing groundwaters from 67 wells completed in the Tertiary sediments, increasing U concentrations in the direction of groundwater flow generally were associated with a maturation of the formation water as evidenced by evolutionary trends in major ion character. The increased U levels probably are associated with leaching as shown by the positive correlation between U concentrations and total dissolved solids (TDS) (r = +0.83). The inverse relationships between TDS and U ARs (r = ?0.73) and U levels and ARs (r = 0.72) indicate that the decay of excess U-234 is related to maturation of the formation water and to sediment leaching along the flowpath. The data are described by a model which incorporates etching, decay and recoil and suggests that aquifer residence time can be estimated from the TDS level.The levels of soluble U in a reducing uraniferous hydrogeologic unit near Crawford, Nebraska are affected by the proximity of the sample collection to ore. In groundwater samples having similar chemistries (Na-SO4 + Cl type), similar Ehs, and collected from a close-knit pattern, U concentrations ranged from 0.01 to 2,037 μg l?1 and ARs ranged from 0.75 to 12.6. This high variability in U levels and ARs is indicative of uranium ore in small areal studies where low ARs almost always are associated with high U concentrations.  相似文献   

14.
Isotopic fractionation as great as 1600% exists between 234U and 238U in spring waters, sediments, and fossils in the Pomme de Terre Valley, southwestern Missouri. The activity ratios of 234U238U in five springs range from 7.2 to 16 in water which has been discharged for at least the past 30,000 years. The anomalies in 234U238U ratio in deep water have potential usefulness in hydrologic investigations in southern Missouri. Clayey units overlying the spring bog sediments of Trolinger Spring are enriched in 230Th relative to their parent 234U by as much as 720%. The results indicate that both preferential displacement via alpha recoil ejection and the preferential emplacement via recoiling and physical entrapment are significant processes that are occurring in the geologic environment.  相似文献   

15.
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.  相似文献   

16.
Extreme U and Pb isotope variations produced by disequilibrium in decay chains of 238U and 232Th are found in calcite, opal/chalcedony, and Mn-oxides occurring as secondary mineral coatings in the unsaturated zone at Yucca Mountain, Nevada. These very slowly growing minerals (mm my−1) contain excess 206Pb and 208Pb formed from excesses of intermediate daughter isotopes and cannot be used as reliable 206Pb/238U geochronometers. The presence of excess intermediate daughter isotopes does not appreciably affect 207Pb/235U ages of U-enriched opal/chalcedony, which are interpreted as mineral formation ages.Opal and calcite from outer (younger) portions of coatings have 230Th/U ages from 94.6 ± 3.7 to 361.3 ± 9.8 ka and initial 234U/238U activity ratios (AR) from 4.351 ± 0.070 to 7.02 ± 0.12, which indicate 234U enrichment from percolating water. Present-day 234U/238U AR is ∼1 in opal/chalcedony from older portions of the coatings. The 207Pb/235U ages of opal/chalcedony samples range from 0.1329 ± 0.0080 to 9.10 ± 0.21 Ma, increase with microstratigraphic depth, and define slow long-term average growth rates of about 1.2-2.0 mm my−1, in good agreement with previous results. Measured 234U/238U AR in Mn-oxides, which pre-date the oldest calcite and opal/chalcedony, range from 0.939 ± 0.006 to 2.091 ± 0.006 and are >1 in most samples. The range of 87Sr/86Sr ratios (0.71156-0.71280) in Mn-oxides overlaps that in the late calcite. These data indicate that Mn-oxides exchange U and Sr with percolating water and cannot be used as a reliable dating tool.In the U-poor calcite samples, measured 206Pb/207Pb ratios have a wide range, do not correlate with Ba concentration as would be expected if excess Ra was present, and reach a value of about 1400, the highest ever reported for natural Pb. Calcite intergrown with opal contains excesses of both 206Pb and 207Pb derived from Rn diffusion and from direct α-recoil from U-rich opal. Calcite from coatings devoid of opal/chalcedony contains 206Pb and 208Pb excesses, but no appreciable 207Pb excesses. Observed Pb isotope anomalies in calcite are explained by Rn-produced excess Pb. The Rn emanation may strongly affect 206Pb-238U ages of slow-growing U-poor calcite, but should be negligible for dating fast-growing U-enriched speleothem calcite.  相似文献   

17.
The 234U/238U alpha activity ratio (AR) was determined in 47 samples of variably uraniferous groundwater from the vicinity of a uranium mill near Cañon City, Colorado. The results illustrate that uranium isotopes can be used to determine the distribution of uranium contamination in groundwater and to indicate processes such as mixing and chemical precipitation that affect uranium concentrations. Highly to moderately contaminated groundwater samples collected from the mill site and land immediately downgradient from the mill site contain more than 100?μg/l of dissolved uranium and typically have AR values in the narrow range of 1.0–1.06. Other samples from the shallow alluvial aquifer farther downgradient from the mill contain 10–100?μg/l uranium and plot along a broad trend of increasing AR (1.06–1.46) with decreasing uranium concentration. The results are consistent with mixing of liquid mill waste (AR≈1.0) with alluvial groundwater of small, but variable, uranium concentrations and AR of 1.3–1.5. In the alluvial aquifer, the spatial distribution of wells with AR values less than 1.3 is consistent with previous estimates of the probable distribution of contamination, based on water chemistry and hydrology. Wells more distant from the area of probable contamination have AR values that are consistently greater than 1.3 and are indicative of little or no contamination. The methodology of this study can be extended usefully to similar sites of uranium mining, milling, or processing provided that local geohydrologic settings promote uranium mobility and that introduced uranium contamination is isotopically distinct from that of local groundwater.  相似文献   

18.
Factors controlling the groundwater transport of U, Th, Ra, and Rn   总被引:1,自引:0,他引:1  
A model for the groundwater transport of naturally occurring U, Th, Ra, and Rn nuclides in the238U and232Th decay series is discussed. The model developed here takes into account transport by advection and the physico-chemical processes of weathering, decay, α-recoil, and sorption at the water-rock interface. It describes the evolution along a flowline of the activities of the238U and232Th decay series nuclides in groundwater. Simple sets of relationships governing the activities of the various species in solution are derived, and these can be used both to calculate effective retardation factors and to interpret groundwater data. For the activities of each nuclide, a general solution to the transport equation has been obtained, which shows that the activities reach a constant value after a distance ϰi, characteristic of each nuclide. Where ϰi is much longer than the aquifer length, (for238U,234U, and232Th), the activities grow linearly with distance. Where gKi is short compared to the aquifer length, (for234Th,230Th,228Th,228Ra, and224Ra), the activities rapidly reach a constant or quasi-constant activity value. For226Ra and222Rn, the limiting activity is reached after 1 km. High δ234U values (proportional to the ratioɛ234Th/W238U) can be obtained through high recoil fraction and/or low weathering rates. The activity ratios230Th/232Th,228Ra/226Ra and224Ra/226Ra have been considered in the cases where either weathering or recoil is the predominant process of input from the mineral grain. Typical values for weathering rates and recoil fractions for a sandy aquifer indicate that recoil is the dominant process for Th isotopic ratios in the water. Measured data for Ra isotope activity ratios indicate that recoil is the process generally controlling the Ra isotopic composition in water. Higher isotopic ratios can be explained by different desorption kinetics of Ra. However, the model does not provide an explanation for228Ra/226Ra and224Ra/226Ra activity ratios less than unity. From the model, the highest222Rn emanation equals 2ɛ. This is in agreement with the hypothesis that222Rn activity can be used as a first approximation for input by recoil (Krishnaswamiet al 1982). However, high222Rn emanation cannot be explained by production from the surface layer as formulated in the model. Other possibilities involve models including surface precipitation, where the surface layer is not in steady-state.  相似文献   

19.
The Opalinus Clay formation in North Switzerland is a potential host rock for a deep underground radioactive waste repository. The distribution of 238U, 234U and 230Th was studied in rock samples of the Opalinus Clay from an exploratory borehole at Benken (Canton of Zurich) using MC-ICP-MS. The aim was to assess the in situ, long-term migration behaviour of 234U in this rock. Very low hydraulic conductivities of the Opalinus Clay, reducing potential of the pore water and its chemical equilibrium with the host rock are expected to render both 238U and 230Th immobile. If U is heterogeneously distributed in the Opalinus Clay, gradients in the supply of 234U from the rock matrix to the pore water by the decay of 238U will be established. Diffusive redistribution separates 234U from its immobile parent 238U resulting in bulk rock 234U/238U activity disequilibria. These may provide a means of estimating the mobility of 234U in the rock if the diffusion rate of 234U is significant compared to its decay rate. Sampling was carried out on two scales. Drilling of cm-spaced samples from the drill-core was done to study mobility over short distances and elucidate possible small-scale lithological control. Homogenized 25-cm-long portions of a 2-m-long drill-core section were prepared to provide information on transport over a longer distance. Variations in U and/or Th content on the cm-scale between clays and carbonate-sandy layers are revealed by β-scanning, which shows that the (dominant) clay is richer in both elements.  相似文献   

20.
To examine the petrogenesis and sources of basalts from the Kolbeinsey Ridge, one of the shallowest locations along the global ridge system, we present new measurements of Nd, Sr, Hf, and Pb isotopes and U-series disequilibria on 32 axial basalts. Young Kolbeinsey basalts (full-spreading rate = 1.8 cm/yr; 67°05′-70°26′N) display (230Th/238U) < 1 and (230Th/238U) > 1 with (230Th/238U) from 0.95 to 1.30 and have low U (11.3-65.6 ppb) and Th (33.0 ppb-2.40 ppm) concentrations. Except for characteristic isotopic enrichment near the Jan Mayen region, the otherwise depleted Kolbeinsey basalts (e.g. 87Sr/86Sr = 0.70272-0.70301, εNd = 8.4-10.5, εHf = 15.4-19.6 (La/Yb)N = 0.28-0.84) encompass a narrow range of (230Th/232Th) (1.20-1.32) over a large range in (238U/232Th) (0.94-1.32), producing a horizontal array on a (230Th/232Th) vs. (238U/232Th) diagram and a large variation in (230Th/238U). However, the (230Th/238U) of the Kolbeinsey Ridge basalts (0.96-1.30) are inversely correlated with (234U/238U) (1.001-1.031). Samples with low (230Th/238U) and elevated (234U/238U) reflect alteration by seawater or seawater-derived materials. The unaltered Kolbeinsey lavas with equilibrium 234U/238U have high (230Th/238U) values (?1.2), which are consistent with melting in the presence of garnet. This is in keeping with the thick crust and anomalously shallow axial depth for the Kolbeinsey Ridge, which is thought to be the product of large degrees of melting in a long melt column. A time-dependent, dynamic melting scenario involving a long, slowly upwelling melting column that initiates well within the garnet peridotite stability zone can, in general, reproduce the (230Th/238U) and (231Pa/235U) ratios in uncontaminated Kolbeinsey lavas, but low (231Pa/235U) ratios in Eggvin Bank samples suggest eclogite involvement in the source for that ridge segment.  相似文献   

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