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1.
Uranium-series mass spectrometric analyses of corals from the uplifted last glacial terraces at Huon Peninsula, Papua New Guinea, that grew from 50,000 years ago to 30,000 years ago show systematically low values of 234U/238U, at the time of coral growth, compared with modern corals. When combined with coral data from other studies a systematic trend emerges indicating shifts in the 234U/238U ratio at times of major glacial-interglacial transitions that involve large variations in sea-levels. From last glacial to Holocene, the rate of change in δ234U is approximately 1‰ per thousand years. The variations in the U budget of the oceans appear to be due to accumulation of excess 234U in near shore areas in anoxic and suboxic sediments, in salt marshes and mangroves, in estuaries, and in continental margins during periods of warm climate and high sea-levels. These near-shore areas are exposed during periods of low sea level resulting in rapid oxidation of U into highly soluble phases. The subsequent release of 234U-enriched uranium into the oceans occurs over a sustained period, in step with rising sea-levels.  相似文献   

2.
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   

3.
The 230Th/234U/238U age dating of corals via alpha counting or mass spectrometry has significantly contributed to our understanding of sea level, radiocarbon calibration, rates of ocean and climate change, and timing of El Nino, among many applications. Age dating of corals by mass spectrometry is remarkably precise, but many samples exposed to freshwater yield inaccurate ages. The first indication of open-system 230Th/234U/238U ages is elevated 234U/238Uinitial values, very common in samples older than 100,000 yr. For samples younger than 100,000 yr that have 234U/238Uinitial values close to seawater, there is a need for age validation. Redundant 230Th/234U/238U and 231Pa/235U ages in a single fossil coral fragment are possible by Multi-Collector Magnetic Sector Inductively Coupled Plasma Mass Spectrometry (MC-MS-ICPMS) and standard anion exchange column chemistry, modified to permit the separation of uranium, thorium, and protactinium isotopes from a single solution. A high-efficiency nebulizer employed for sample introduction permits the determination of both 230Th/234U/238U and 231Pa/235U ages in fragments as small as 500 mg. We have obtained excellent agreement between 230Th/234U/238U and 231Pa/235U ages in Barbados corals (30 ka) and suggest that the methods described in this paper can be used to test the 230Th/234U/238U age accuracy.Separate fractions of U, Th, and Pa are measured by employing a multi-dynamic procedure, whereby 238U is measured on a Faraday cup simultaneously with all minor isotopes measured with a Daly ion counting detector. The multi-dynamic procedure also permits correcting for both the Daly to Faraday gain and for mass discrimination during sample analyses. The analytical precision of 230Th/234U/238U and 231Pa/235U dates is generally better than ±0.3% and ±1.5%, respectively (2 Relative Standard deviation [RSD]). Additional errors resulting from uncertainties in the decay constant for 231Pa and from undetermined sources currently limit the 231Pa/235U age uncertainty to about ±2.5%. U isotope data and 230Th/234U/238U ages agree with National Institute of Standards and Technology (NIST) reference materials and with measurements made by Thermal Ionization Mass Spectrometry (TIMS) in our laboratory.  相似文献   

4.
Wet climatic episodes are known to have prevailed in the Egyptian Sahara several times during the late Quaternary, most recently during the Holocene 8000 yr ago. Earlier wet episodes have been recognized as having occurred during the past 300,000 yr and have been dated by U-series methods in speleothems and in lake travertines. We show here that the times of enhanced groundwater movement can also be determined by 230Th/234U dating of secondary U in ores of uranium, iron, and phosphate. We also present evidence that such acceleration of groundwater movements is indicated by relatively low 234U/238U activity ratios in the secondary uranium. Our new data show that pluvial periods in Egypt occurred during marine oxygen isotope stages 4, 5, 6, and 7 and therefore are consistent with the view that the wet episodes are the results of migration of the tropical monsoonal belt driven primarily by the 23,000-yr precession cycle of the Milankovich curve, modulated by the 100,000-yr eccentricity cycle.  相似文献   

5.
A simple, reliable, and high-performance method has been proposed for direct determination of the isotopic composition of authigenic uranium in silica lacustrine sediments. The method is based on studying the kinetics of the selective extraction of authigenic uranium from sediments with weak solutions of ammonium hydrocarbonate followed by the ICP-MS analysis of the nuclides. To estimate the contamination of authigenic uranium by terrigenous one, the contents of 232Th and some other clastogenic elements in the extracts were measured simultaneously. The selectivity of extraction of authigenic uranium from the sediments treated with a 1% NH4HCO3 solution appeared to be no worse than 99%. The method was used to analyze the isotopic composition of authigenic uranium at several key horizons of a core dated before. The measurements directly prove that the 234U/238U values in Baikal water varied depending on climate, which contradicts the previous statements. The measured 234U/238U ratios in paleo-Baikal water match the values reconstructed from isotopic data for total uranium in the sediments on the supposition that the U/Th ratio is constant in the terrigenous part of the sediment. Direct experimental determination of total and authigenic nuclides in sediments enhances the potentiality of the method for absolute 234U-230Th dating of carbonate-barren lacustrine sediments, including those from Lake Baikal, within the intervals corresponding to the periods of glaciation, where the sediments contain a large fraction of terrigenous component. Given the fractions of terrigenous and authigenic uranium are accurately determined, we have an opportunity to study the variability of the sources of terrigenous matter and to refine the previous model for reconstructing the climate humidity in East Siberia.  相似文献   

6.
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   

7.
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   

8.
Uranium-series disequilibrium dating of island phosphate deposits is evaluated in terms of known associated coral ages, uranium geochemistry, and stratigraphic sequences as well as the concordance between the geochronometers 234U/238U, 230Th/234U and 226Ra/238U. U(VI) is the predominant oxidation state of uranium in island phosphorites and by analogy to the youngest surficial deposits, most of the uranium initially bound is in the form of U(VI) sorbed by surfaces from seawater. Insular deposits contain more organic matter than even very young ocean floor samples and this leads to a greater probability of reduction of available recoil uranium than occurs in marine deposits. As a consequence, R(VI) ? R(T) ? R(VI), where R represents the 234U/238U activity ratio. This situation is completely opposite from that observed for marine-origin phosphorites. We determined that a fraction of U(VI) in ancient insular phosphorites is very labile and lost to alkaline carbonate solutions with a uranium activity ratio even more depleted in 234U than the bulk R(VI).Most younger samples appear to have no more discordance between 234U/238U, 230Th/234U and 226Ra/238U than marine phosphorites of similar apparent age. Young, surficial atoll-rim apatite cements and unconsolidated phosphorites date in the range of 1500–8000 years B.P., consistent with the concept of partial submergence of low-lying coral islands prior to 2000 years B.P. Sub-surficial samples in the same environment date older at about 20,000 years B.P. Violation of the closed system assumption occurs in at least 6 out of 13 ancient (> 800,000 year) samples. Uranium-series disequilibrium dating of insular apatite shows some promise as a recorder of climatic/sea level events, but the assumptions necessary for valid ages must be carefully evaluated for each occurrence.  相似文献   

9.
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   

10.
In this paper, we evaluate the factors that influence the accuracy of lead (Pb)-isotopic ages of meteorites, and may possibly be responsible for inconsistencies between Pb-isotopic and extinct nuclide timescales of the early Solar System: instrumental mass fractionation and other possible analytical sources of error, presence of more than one component of non-radiogenic Pb, migration of ancient radiogenic Pb by diffusion and other mechanisms, possible heterogeneity of the isotopic composition of uranium (U), uncertainties in the decay constants of uranium isotopes, possible presence of “freshly synthesized” actinides with short half-life (e.g. 234U) in the early Solar System, possible initial disequilibrium in the uranium decay chains, and potential fractionation of radiogenic Pb isotopes and U isotopes caused by alpha-recoil and subsequent laboratory treatment. We review the use of 232Th/238U values to assist in making accurate interpretations of the U-Pb ages of meteorite components. We discuss recently published U-Pb dates of calcium-aluminum-rich inclusions (CAIs), and their apparent disagreement with the extinct nuclide dates, in the context of capability and common pitfalls in modern meteorite chronology. Finally, we discuss the requirements of meteorites that are intended to be used as the reference points in building a consistent time scale of the early Solar System, based on the combined use of the U-Pb system and extinct nuclide chronometers.  相似文献   

11.
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   

12.
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   

13.
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   

14.
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   

15.
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   

16.
A radiometric calibration of the SPECMAP timescale   总被引:1,自引:0,他引:1  
The astronomical theory of climate change asserts that Earth's climate is affected by changes in its orbit, which vary the seasonal and latitudinal distribution of solar radiation. This theory is the basis of the orbitally tuned SPECMAP timescale. A key constraint for this important chronology was the mid-point of the Penultimate Deglaciation, initially dated to 127,000 years ago. Recent work suggests this event may be considerably older, casting doubt on the astronomical theory, the SPECMAP timescale, and the accuracy of orbitally tuned chronologies. Difficulties with U/Th coral dating of sea-level events have impeded progress on this problem, because most corals are not closed systems. Here, we use a new approach to U/Th dating that corrects for open-system behavior and produces a sea-level curve of sufficient resolution to confidently correlate with SPECMAP over the last 240,000 years, permitting a reassessment of both this critical chronology and a central tenet of climate change theory. High-precision ages for 24 oxygen isotope events provide a 240,000-year chronology for marine δ18O records that is independent of orbital tuning assumptions. Although there appear to be significant differences between the radiometric and orbitally tuned timescales near the lastglacial maximum and at the Marine Isotope Stage 7/6 boundary, a comparison of radiometric and SPECMAP ages for identical isotope events suggest that the SPECMAP timescale is quite accurate and that its errors were, in general, overestimated. Despite suborbital complexity, orbital cyclicity is clearly evident in our record. High-amplitude sea-level oscillations at periods greater than 20,000 years are very close in phase to summer insolation in the Northern Hemisphere. Although sea-level changes cannot be uniquely tied to a specific season or latitude of insolation forcing, the simplest explanation is that long-period, high-amplitude sea-level change is linked to Northern Hemisphere insolation forcing. These results validate the principles of orbital tuning and suggest such timescales are generally robust.  相似文献   

17.
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   

18.
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   

19.
We investigated the effects of diagenetic alteration (dissolution, secondary aragonite precipitation and pore filling) on the distribution of U in live and Holocene coral skeletons. For this, we drilled into large Porites lutea coral-heads growing in the Nature Reserve Reef (NRR), northern Gulf of Aqaba, a site close to the Marine Biology Laboratory, Elat, Israel, and sampled the core material and porewater from the drill-hole. In addition, we sampled Holocene corals and beachrock aragonite cements from a pit opened in a reef buried under the laboratory grounds. We measured the concentration and isotopic composition of U in the coral skeletal aragonite, aragonite cements, coral porewater and open NRR and Gulf of Aqaba waters.Uranium concentration in secondary aragonite filling the skeletal pores is significantly higher than in primary biogenic aragonite (17.3 ± 0.6 compared to 11.9 ± 0.3 nmol · g−1, respectively). This concentration difference reflects the closed system incorporation of uranyl tri-carbonate into biogenic aragonite with a U/Ca bulk distribution coefficient (KD) of unity, versus the open system incorporation into secondary aragonite with KD of 2.4. The implication of this result is that continuous precipitation of secondary aragonite over ∼1000 yr of reef submergence would reduce the coral porosity by 5% and can produce an apparent lowering of the calculated U/Ca - SST by ∼1°C and apparent age rejuvenation effect of 7%, with no measurable effect on the calculated initial U isotopic composition.All modern and some Holocene corals (with and without aragonite cement) from Elat yielded uniform δ234U = 144 ± 5, similar to the Gulf of Aqaba and modern ocean values. Elevated δ234U values of ∼180 were measured only in mid-Holocene corals (∼5000 yr) from the buried reef. The values can reflect the interaction of the coral skeleton with 234U-enriched ground-seawater that washes the adjacent granitic basement rocks.We conclude that pore filling by secondary aragonite during reef submergence can produce small but measurable effects on the U/Ca thermometry and the U-Th ages. This emphasizes the critical importance of using pristine corals where the original mineralogy and porosity are preserved in paleooceanographic tracing and dating.  相似文献   

20.
Because stalagmites are enriched in 234U beyond the equilibrium value at the time of deposition, they are potentially datable by measuring their progress toward equilibrium. Procedures for uranium-thorium and uranium disequilibrium dating of speleothems were developed, making use of alpha spectrometry for thorium determinations and mass spectrometry for uranium determinations. The stalagmites tested were generally beyond the age range of the U-Th age dating method and, as a result, 234U/238U ratios provided the most useful dating technique. The estimated age range for a stalagmite from Blanchard Springs is 135,000 to 785,000 years BP with an interval of slow or suspended growth from about 320,000 to 570,000 years BP.  相似文献   

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