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1.
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.  相似文献   

2.
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   

3.
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.  相似文献   

4.
U-modeled groundwater residence times were estimated by changes in 234U/238U activity ratio (AR) and U content of groundwaters from Poços de Caldas city situated at the Poços de Caldas alkaline massif, Brazil. The estimated ages are more realistic than others generated by the use of hydraulic conductivity data and available information about the weathering rate of rocks in the plateau. The 234U/238U AR and reciprocal of the dissolved U-content data also defined a ternary plot that allowed the calculation of the relative volume of three source waters for the mixed water. Such U-isotopes modeling for mixing calculations indicated that the dominant phase (68%) in the mixture is thermal.  相似文献   

5.
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.  相似文献   

6.
This study investigates U-series, Sr isotopes, major and trace elements in a chalk aquifer system located in Eastern France. Soil and rock samples were collected along depth profiles down to 45 m in four localities as an attempt to investigate the weathering processes in the soil, the unsaturated zone and the saturated zone of the aquifer. Interstitial water was extracted from soils and rocks by a centrifugation technique. U-series offer a powerful tool to calculate weathering rates because the relative mobility of the U- and Th-isotopes can be precisely measured and it does not require the determination of a reference state as in other approaches. As expected, the data show very large mobile element depletion in the soil with large 230Th excess relative to 238U, while the rocks show more limited but not insignificant mobile element depletion. The U-series data have been used to constrain weathering rates based on a 1-D reactive transport model. Weathering rates in the near surface are about 10–100 times faster than at depth. However, when integrated over the depth of the cores, including the unsaturated and the saturated zones, this underground weathering represents more than 30% of the total weathering flux, assuming congruent dissolution of carbonates. The (234U/238U) ratios in interstitial water are consistent with solid samples showing 234U depletion near the surface and an excess 234U at depth. A leaching experiment performed on chalk shows that the excess 234U in natural waters percolating through carbonate rocks results both from preferential 234U leaching and direct recoil in the interstitial water. A new approach was used to derive the recoil ejection factor based on BET measurements and the fractal dimension of chalk surface. Consideration of preferential leaching and recoil allows a more accurate modeling of weathering rates.  相似文献   

7.
The radioactivity due to 238U and 234U in three aquifer systems occurring within the Paraná sedimentary basin, South America, has been investigated. Uranium is much less dissolved from fractured igneous rocks than from the porous sedimentary rocks as indicated by the U-mobility coefficients between 7.6 × 10?6 and 1.2 × 10?3 g cm?3. These values are also compatible with the U preference ratios relative to Na, K, Ca, Mg and SiO2, which showed that U is never preferentially mobilized in the liquid phase during the flow occurring in cracks, fissures, fractures and faults of the igneous basaltic rocks. Experimental dissolution of diabase grains on a time-scale laboratory has demonstrated that the U dissolution appeared to be a two-stage process characterized by linear and second-order kinetics. The U dissolution rate was 8 × 10?16 mol m?2 s?1 that is within the range of 4 × 10?16–3 × 10?14 mol m?2 s?1 estimated for other rock types. The 234U/238U activity ratio of dissolved U in solutions was higher than unity, a typical result expected during the water–rock interactions when preferential 234U-leach from the rock surfaces takes place. Some U-isotopes data allowed estimating 320 ka for the groundwater residence time in a sector of a transect in São Paulo State. A modeling has been also realized considering all U-isotopes data obtained in Bauru (35 samples), Serra Geral (16 samples) and Guarani (29 samples) aquifers. The results indicated that the Bauru aquifer waters may result from the admixture of waters from Guarani (1.5 %) and Serra Geral (98.5 %) aquifers.  相似文献   

8.
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   

9.
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   

10.
Dissolved uranium concentration and 234U/238U activity ratio have been measured in two distinctly different Indian drainage systems: the Yamuna headwaters in the Himalaya and the Chambal river system in the plains to study the weathering and mobility of uranium in these watersheds. The dissolved uranium in the Chambal river system ranges from 0.2 to 1.74 μg L−1 during September (tail end of monsoon), whereas in the Yamuna river system, its concentration varies from 0.1 to 3.18 μg L−1 during October (post-monsoon) and from 0.09 to 3.61 μg L−1 in June (summer). In the Yamuna main stream, uranium is highest at its source and decreases steadily along its course, from 3.18 μg L−1 at Hanuman Chatti to 0.67 μg L−1 at Batamandi, at the base of the Himalaya. This decrease results mainly from mixing of the Yamuna mainstream with its tributaries, which are lower in uranium. The high concentration of uranium at Hanuman Chatti is derived from weathering of the Higher Himalayan Crystalline series (HHC) and associated accessary minerals, which may include uranium-mineralised zones. The 234U/238U activity ratios in the samples from the Chambal watershed are in the range of 1.15±0.05 to 1.67±0.04; whereas in the Yamuna the ratios vary from 0.95±0.03 to 1.56±0.07, during post-monsoon and from 0.98±0.01 to 1.30±0.03, during summer. The relatively high 234U/238U activity ratios in the Yamuna system are in its tributaries from the lower reaches viz., the Amlawa, Aglar, Bata, Tons and the Giri. It is estimated that ~9×103 and ~12 × 103 kg of dissolved uranium are transported annually from the Yamuna at Batamandi and the Chambal at Udi, respectively. This corresponds to uranium weathering rates of 0.9 and 0.09 kg U km−2 y−1 in the basins of the Yamuna and the Chambal headwaters. This study confirms that uranium weathering rate in the Himalaya is far in excess (by about an order of magnitude) of the global average value of ~0.08 kg U km−2 y−1.  相似文献   

11.
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 238U238U 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 234U238U activity ratio of 1.20 ± 0.06ismissing. The residence time of uranium isotopes in the oceans estimated from the 238U concentration and the 234U238U 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.  相似文献   

12.
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.  相似文献   

13.
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.  相似文献   

14.
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.  相似文献   

15.
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   

16.
The radioactive and physical characteristics of Syrian hot waters were studied. The concentration of uranium, its daughters and the 234U/238U-activity ratios in the hot waters were measured by gamma and alpha ray spectroscopy. The 234U/238U-activity ratios showed that uranium in Syrian hot waters are in an equilibrium state. Some anomalous observations of these ratios were explained by former leaching of the uranium from Cretaceous phosphates by underground water. Also, the results showed that the temperature of the studied hot waters was independent of the contained radioelements. The temperature of hot waters is explained by the passing of these waters near the hot spot or by the relationship between the geological deposit of the aquifer rocks and the waters rather than the contents of the radioelements.  相似文献   

17.
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   

18.
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.  相似文献   

19.
The economic iron ore deposits of Egypt are located at Bahariya Oasis in the Lower Middle Eocene limestone. The main iron minerals are goethite, hematite, siderite, pyrite, and jarosite. Manganese minerals are pyrolusite and manganite. Gangue minerals are barite, glauconite, gibbsite, alunite, quartz, halite, kaolinite, illite, smectite, palygorskite, and halloysite. Geochemical comparison between the ore and the Nubia sandstone showed that the ore is depleted in the residual elements (Al, Ti, V, and Ni) and enriched in the mobile elements (Fe, Mn, Zn, Ba, and U) which indicates that the Bahariya iron ore is not a lateritic deposit despite the deep weathering in this area. On the other hand, the Nubia sandstone showed depletion in the mobile elements, which demonstrates the leaching process in the Nubia Aquifer. The presence of such indicator minerals as jarosite, alunite, glauconite, gibbsite, palygorskite, and halloysite indicate that the ore was deposited under strong acidic conditions in fresh water.Isotopic analyses of the uranium in the amorphous and crystalline phases of the ore, in the country rocks, and dissolved in the Nubia Aquifer water, all support the conclusion that U and Fe were precipitated together from warm ascending groundwater. U and Fe display strong co-variation in the ore, and the 234U/238U activity ratio of the newly precipitated U in the country rock and the leached component of U in the groundwater are identical. There is only slightly more uranium in the amorphous phase than in the crystalline and only a slightly lower 234U/238U activity ratio, suggesting that the iron in the two phases have a similar origin. Comparison of the excess 234U in the water and in the total ore leads to the conclusion that the precipitation of the U, and by inference the iron, occurred within the last million years. However, that both precipitation and leaching of U have occurred over the last 300,000 years is evidenced by the extreme 230Th/234U disequilibria observed in some of the samples. Some of the amorphous depositional events have been very recent, perhaps within the last 10,000 years.  相似文献   

20.
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.  相似文献   

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