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1.
Abundances of 238U, 234U, 232Th, 226Ra, 228Ra, 224Ra, and 222Rn were measured in groundwaters of the Ojo Alamo aquifer in northwest New Mexico. This is an arid area with annual precipitation of ∼22 cm. The purpose was to investigate the transport of U-Th series nuclides and their daughter products in an old, slow-moving groundwater mass as a means of understanding water-rock interactions and to compare the results with a temperate zone aquifer. It was found that 232Th is approximately at saturation and supports the view of Tricca et al. (2001) that Th is precipitated irreversibly upon weathering, leaving surface coatings of 232Th and 230Th on aquifer grains. Uranium in the aquifer waters has very high [234U/238U] ∼ 9 and low 238U concentrations. These levels can be explained by low weathering rates in the aquifer (w238U ∼ 2 × 10−18 to 2 × 10−17s−1) using a continuous flow, water-rock interaction model. The Ra isotopes are roughly in secular equilibrium despite their very different mean lifetimes. The 222Rn and 228Ra isotopes in the aquifer correspond to ∼10% of the net production rate of the bulk rock. This is interpreted to reflect an earlier formed irreversible surface coating of Th that provides Ra and Rn to the aquifer waters. The surface waters that appear to be feeding the aquifer have low [234U/238U] and high 238U concentrations. The flow model shows that it is not possible to obtain the high [234U/238U] and low [238U] values in the aquifer from a source like the present vadose zone input. It follows that the old aquifer waters studied cannot be fed by the present vadose zone input unless they are greatly diluted with waters with very low U concentrations. If the present sampling of vadose zone sources is representative of the present input, then this requires that there was a major change in water input with much larger rainfall some several thousand years ago. This may represent a climatic change in the Southwest.  相似文献   

2.
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   

3.
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.  相似文献   

4.
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   

5.
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   

6.
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   

7.
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   

8.
Stilbite from Malmberget and Svappavara is part of hydrothermal mineral assemblages occupying regionally occurring open Palaeoproterozoic fractures in northern Sweden. At these locations, stilbite is characterized by Pbrad excess relative to U and by activity ratios of [234U]/[238U] > 1 and [230Th]/[238U] > 1. The activity disequilibrium requires a disturbance of the U-Th systematics within the last one million years. Leaching and infiltration experiments on Malmberget stilbite demonstrate: (i) preferential leaching in the order Pb >U >Th and uptake in the order Pb > U, and (ii) isotopic fractionation of U by preferential mobilization of 238U and 235U relative to 234U. Stepwise-leaching further indicates that the bulk of U is hosted in the channel sites of stilbite. The Th-U disequilibrium systematics observed in untreated Malmberget and Svappavara stilbite can be explained by: (1) addition of U with [234U]/[238U] > 1 from a fluid, or alternatively (2) loss of U from a two-component system, consisting of a component that is “open” or accessible and a component that is “closed” or inaccessible to mobilization. U addition requires a multistage history involving multiple gain or loss of U and/or Pb. In contrast, U loss does not necessarily require multistage processes but can also be explained by preferential removal of 238U (and 235U) relative to recoiled daughter isotopes such as 234U, 230Th, and 206Pb (and 207Pb) during a single event. Such a behavior could be obtained if the recoiled daughter isotopes of channel-sited uranium are implanted into the crystal lattice and, in such a way, become less mobile than their parent isotopes. This case implies an open-system behavior for ions in the channel sites and a closed-system behavior for ions in the silicate framework of stilbite. Each α-recoil directly or indirectly, i.e., through its recoil cascade, damages the silicate framework. Subsequent (continuous) low-temperature annealing of the damaged stilbite lattice could trap the recoiled daughter isotopes in the repaired crystal lattice or sealed-off channels. Such immobile recoiled material can, in part, represent the “closed” component of the system. This model can account for all observations regarding the Th-U-Pb systematics, including the Th-U disequilibrium systematics, the similarity in Th/U as deduced from Th-U disequilibrium and Pb isotope data, and the excess of radiogenic Pb (208Pb-parents also had been multiply recoiled). These two contrasting explanations involve either multistage or multicomponent systems. They do not permit the derivation of an accurate age.  相似文献   

9.
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   

10.
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   

11.
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.  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.
U-series disequilibria measured in waters and rocks from a chalk aquifer in France have been used as an analog for long-term radionuclide migration. Drill core samples from a range of depths in the vadose zone and in the saturated zone, as well as groundwater samples were analyzed for 238U, 234U, 232Th and 230Th to determine transport mechanisms at the water/rock interface and to quantify parameters controlling the migration of radionuclides. Isotope measurements in rocks were done by TIMS, whereas (234U/238U) and (230Th/232Th) activity ratios in water samples were measured by multi-collector-ICP-MS. Both depletion and enrichment in 234U relative to 238U were observed in carbonate rock samples resulting from chemical weathering in the unsaturated zone and calcite precipitation in the zone of water-table oscillation, respectively. The correlation between (230Th/232Th) activity ratios and 87Sr/86Sr ratios found in the chalk samples indicates that thorium is mainly contained in a minor silicate phase whose abundance is variable in chalk samples. Water samples are all characterized by (234U/238U) > 1 resulting from α-recoil effect of 234Th. Groundwaters are characterized by a more radiogenic signature in 87Sr/86Sr than the rocks. Moreover, (230Th/232Th) activity ratios in the waters are lower than in the rocks, and increase with distance from the water divide, which suggests that Th transport is controlled by colloids formed during water infiltration in the soil. A 1-D transport model has been developed in order to constrain the U-series nuclide transport considering a transient behavior of radionuclides in the aquifer and a time-dependent composition for the solid phase. This model permits a prediction of the time scale of equilibration of the system, and an estimation of parameters such as weathering rate, distribution coefficients and α-recoil fractions. Retardation factors of 10-35 and from 1 × 104 to 2 × 105 were predicted for U and Th, respectively, and can be used to predict the migration of radionuclides released as contaminants in the environment. At the scale of our watershed (∼32 km2), a characteristic migration time from recharge to riverine discharge of 200-600 yr for U and 0.2-3.7 Myr for Th was obtained.  相似文献   

14.
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   

15.
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   

16.
The Water–Sediment Regulation Scheme (WSRS) is an important water conservancy project in the Yellow River basin, which is usually operated annually from June to July to control water and sediment release from the Xiaolangdi Reservoir in the middle reaches. As a greatly concentrated period of delivering terrigenous materials from the Yellow River to the sea, the WSRS can serve as a natural laboratory to examine the geochemical behavior of elements during their transport along the river. Uranium isotopes (234U and 238U) were measured in Yellow River waters at stations Xiaolangdi (located in the middle reaches of the Yellow River) and Lijin (the last hydrologic station near the Yellow River estuary) during the WSRS 2012. Compared with station Xiaolangdi, dissolved uranium concentration at station Lijin was markedly higher, showing a significant impact from the WSRS. Budget calculation for dissolved uranium during the WSRS indicated that two major sources of new added dissolved uranium in the section of the Yellow River between Xiaolangdi and Lijin: suspended particles (46%) and porewater of bottom sediment (45%). The flux of dissolved uranium from the Yellow River to the sea was estimated to be 2.40 × 107 g during the WSRS 2012.  相似文献   

17.
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   

18.
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   

19.
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   

20.
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   

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