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1.
226Ra, 228Ra and Ba distributions as well as 228Ra/226Ra and 226Ra/Ba ratios were measured in seawater, suspended and sinking particles at the DYFAMED station in the Western Mediterranean Sea at different seasons of year 2003 in order to track the build-up and fate of barite through time. The study of the 228Raex/226Raex ratios (Raex = Ra activities corrected for the lithogenic Ra) of suspended particles suggests that Baex (Baex = Ba concentrations corrected for the lithogenic Ba, mostly barite) formation takes place not only in the upper 500 m of the water column but also deeper (i.e. throughout the mesopelagic layer). Temporal changes in the 228Raex/226Raex ratios of sinking particles collected at 1000 m depth likely reflect changes in the relative proportion of barite originating from the upper water column (with a high 228Ra/226Ra ratio) and formed in the mesopelagic layer (with a low 228Ra/226Ra ratio). 228Raex/226Raex ratios measured in sinking particles collected in the 1000 m-trap in April and May suggest that barite predominantly formed in the upper water column during that period, while barite found outside the phytoplankton bloom period (February and June) appears to form deeper in the water column. Combining ratios of both the suspended and sinking particles provides information on aggregation/disaggregation processes. High 226Raex/Baex ratios were also found in suspended particles collected in the upper 500 m of the water column. Because celestite is expected to be enriched in Ra [Bernstein R. E., Byrne R. H. and Schijf J. (1998) Acantharians: a missing link in the oceanic biogeochemistry of barium. Deep-Sea Res. II45, 491-505], acantharian skeletons may contribute to these high ratios in shallow waters. The formation of both acantharian skeletons and barite enriched in 226Ra may thus contribute to the decrease in the dissolved 226Ra activity and 226Ra/Ba ratios of surface waters observed between February and June 2003 at the DYFAMED station.  相似文献   

2.
Measurements were made of the 226Ra/223Ra activity ratio in ground waters obtained from drill holes in the vicinity of uranium mineralization in northern Saskatchewan where certain hydrologic parameters, specifically ground-water velocity and direction, had been determined. The results show that it is possible to approximate the distance from a ground-water sampling point to the area of mineralization owing to differences in the half lives of the two radium nuclides.The theoretical basis for the determination of the distances is explained.  相似文献   

3.
In order to investigate radioactive decay of 130Ba and 132Ba which have half-lives on the order 1020-1021 a, the isotopic composition of xenon has been measured in 3.5 Ga barite of the Dresser Formation, Pilbara, Western Australia. The analyzed samples were collected at about 86 m depth from a diamond drill core (Pilbara Drilling Project). The fact that the sample has been shielded from modern cosmic ray exposure reduces the number of potentially interfering production pathways, simplifying interpretation of the Xe isotope spectrum. This spectrum is clearly distinct from that of either modern or ancient atmospheric Xe. A strong excess of 130Xe is identified, as well as other isotopic excursions which are attributed to mass-dependent isotopic fractionation and contributions from products of uranium fission. The mass-dependent fractionation, estimated at 2.1 ± 0.3% amu−1, can be accounted for by mutual diffusion and Rayleigh distillation during barite formation that is consistent with geological constraints. After correction for mass-dependent fractionation, the concentrations of fissiogenic Xe isotopes demonstrate that the U-Xe isotope system has remained closed over 3.5 Ga. From the excess of 130Xe, the two successive electron capture half life of this isotope is estimated at 6.0 ± 1.1 × 1020 a, which is 3.4 times faster than previously estimated (Meshik et al., 2001). We could not find evidence of 132Ba decay within our Xe isotope spectra.  相似文献   

4.
The geochemistry of Ba, Ra, Th, and U and the potential of using 226Ra/Ba ratios as an alternative dating method are explored in modern and Holocene marine mollusc shells. Five modern shells of the Antarctic scallop Adamussium colbecki collected from the present day beach and six radiocarbon dated specimens from Holocene beach terraces of the Ross Sea region (Antarctic) between 700 and 6100 calibrated yr BP old have been analysed by mass spectrometry. In clean shells 226Ra concentrations and 226Ra/Ba ratios show a clear decrease with increasing age, suggesting the possibility of 226Ra dating. Limiting factors for such dating are Ba and 226Ra present in surface contaminants, and ingrowth of 226Ra from U present within the shell. Surface contamination is difficult to clean off entirely, but moderate levels of residual contamination can be corrected using 232Th. Sub-samples from the same shell with different proportions of contamination form a mixing line in a 226Ra/Ba-232Th/Ba graph, and the 226Ra/Ba of the pure shell can be derived from the intercept on the 226Ra/Ba axis. Contaminant corrected 226Ra/Ba ratios of late-Holocene 14C-dated samples fall close to that expected from simple 226Ra excess decay from seawater 226Ra/Ba values. 226Ra ingrowth from U incorporated into the shell during the lifetime of the mollusc can be corrected for. However, the unknown timing of post mortem U uptake into the shell makes a correction for 226Ra ingrowth from secondary U difficult to achieve. In the A. colbecki shells, 226Ra ingrowth from such secondary U becomes significant only when ages exceed ∼2500 yr. In younger shells, 226Ra/Ba ratios corrected for surface contamination provide chronological information. If evidence for a constant oceanic relationship between 226Ra and Ba in the ocean can be confirmed for that time scale, the 226Ra/Ba chronometer may enable the reconstruction of variability in sea surface 14C reservoir ages from mollusc shells and allow its use as a paleoceanographic tracer.  相似文献   

5.
《Applied Geochemistry》2000,15(3):311-325
Barium/Sr and Ca/Sr ratios have been used to model the relative importance of different sources of stream water. Major and trace element concentrations together with 87Sr/86Sr ratios were measured in precipitation, soil water, groundwater and stream water in a small (9.4 km2) catchment in northern Sweden. The study catchment is drained by a first order stream and mainly covered with podzolized Quaternary till of granitic composition. It is underlain by a 1.8 Ga granite. A model with mixing equations used in an iterative mode was developed in order to separate the stream water into 3 subsurface components: soil water, shallow groundwater, and deep groundwater. Contributions from precipitation are thus not included in the model. This source may be significant for the stream water generation, but it does not interfere with the calculations of the relative contributions from the subsurface components. The results show that the deep groundwater constitutes between 5 and 20% of the subsurface water discharge into the stream water. The highest values of the deep groundwater fraction occur during base flow. Soil water dominates during snowmelt seasons, whereas during base flow it is the least important fraction. Soil water accounts for 10–100% of the subsurface water discharge into the stream water. Shallow groundwater accounts for up to 80% of the subsurface water discharge with the lowest values at peak discharge during snowmelt seasons and the highest values during base flow. The validity of the model was tested by comparing the measured 87Sr/86Sr ratios in the stream water with the 87Sr/86Sr ratios predicted by the model. There was a systematic difference between the measured and modelled 87Sr/86Sr ratios which suggests that the fraction of soil water is overestimated by the model, especially during spring flood. As a consequence of this overestimation of soil water the amount of shallow groundwater is probably underestimated during this period. However, it is concluded that the differences between measured and predicted values are relatively small, and that element ratios are potentially effective tracers for different subsurface water flowpaths in catchments.  相似文献   

6.
A mathematical and computer model for the transport and transformation of solute contaminants through a soil column from the surface to the groundwater is presented. The model simulates selenium species such as selenate, selenite, and selenomethionine as well as pesticides and nitrogen. This model is based on the mass balance equation including convective transport, dispersive transport, surface adsorption, oxidation and reduction, volatilization, chemical and biological transformation. The governing equations are solved numerically by the method of implicit finite difference. The simulation results are in good agreement with measured values. The major finding in the present study indicates that as the time of simulation increases, the concentration of different selenium species approaches the measured values.  相似文献   

7.
Stratiform barite deposits (SB) and vein Pb-Zn barite deposits (VB) are known in a rift basin in central Guangxi. The former is hosted in the Upper Devonian chert beds and the latter occurs in the Middle and Lower Devonian neritic sediments. The two types of mineralization are believed to have a common origin as evidenced by the following observations: (1) Spatially, they are closely associated with each other. (2) They possess a basic similarity, but also show systematic variations from VB to SB in terms of ore composition, structural and textural features, temperature of mineralizing solutions, country rocks and alteration. (3) Their δ34S values are more similar to the average value of marine sulfate in Late Devonian than to that in Early Devonian. A model for thermal water deposition has been proposed to illustrate the genesis of these deposits.  相似文献   

8.
The fate of dissolved material delivered to the coastal ocean depends on its reactivity and the rate at which it is mixed offshore. To measure the rate of exchange of coastal waters, we employ two short-lived radium isotopes,223Ra and224Ra. Along the coast of South Carolina, shore-perpendicular profiles of223Ra and224Ra in surface waters show consistent gradients which may be modeled to yield eddy diffusion coefficients of 350–540 m2s−1. Coupling the exchange rate with offshore concentration gradients yields estimates of offshore fluxes of dissolved materials. For systems in steady state, the offshore fluxes must be balanced by new inputs from rivers, groundwater, sewers or other sources. Two tracers that show promise in evaluating groundwater input are barium and226Ra. These tracers have high relative concentrations in the fluids and low-reactivity in the coastal ocean. Applying the eddy diffusion coefficients to the offshore gradient of226Ra concentration provides an estimate of the offshore flux of226Ra. Measuring the concentrations of226Ra in subsurface fluids provides an estimate of the fluid flux necessary to provide the226Ra. These estimates indicate that the volume of groundwater required to support these fluxes is of the order of 40% of the surface water flow.  相似文献   

9.
The Yucatan Peninsula consists of a karstic terrain that allows the aquifer to directly recharge from rainfall. Due to the various dissolution/precipitation reactions occurring during groundwater flow, the groundwater discharge in the coastal zone becomes a source of trace elements including Ba. The aim of this study was to use the coralline Ba/Ca record as a proxy of precipitation under the consideration that rainfall rates vary at inter-annual time scales. Annual Ba/Ca ratios, both the total content (Ba/CaTC) and the Ca-substitutive fraction (Ba/CaCaF), were quantified in a 52-a old coral colony of Montastraea annularis from the Punta Nizuc Reef, Mexican Caribbean. Average Ba/CaTC (5.90 ± 0.56 μmol/mol) was ∼20% higher than Ba/CaCaF (4.85 ± 0.33 μmol/mol) indicating that Ba is also incorporated in other fractions. Correlation between annual precipitation and Ba/CaTC time-series is significant (r = 0.77, p < 0.05), allowing the use of the Ba/CaTC ratio as a proxy of precipitation, and hence, enabling the reconstruction of precipitation patterns through time. Likewise, the Ba/CaCaF ratio can be used for the reconstruction of dissolved Ba in coastal seawater.  相似文献   

10.
The 18O16O ratios of some New Zealand peat, lignite and coal samples were measured and compared with those of various coal precursors (cellulose, lignin and plant resins). The results showed that the major source of oxygen in all cases (except that of high rank coal) was from cellulose with the contribution from lignin and plant resins being insignificant.  相似文献   

11.
本文运用弹性理论分析了顶空型与顶实型陷落柱压实应力的差异,利用Griffith理论分析了陷落柱活化的判据,认为顶空型陷落柱比顶实陷落柱更易于活化导水.  相似文献   

12.
Doklady Earth Sciences - The paper discusses the results of an experiment conducted in the Sea of Japan in March 2016 on an acoustic track 194 km long in winter hydrological conditions. The most...  相似文献   

13.
Gu  Hongyu  Ni  Huayong  Ma  Fengshan  Liu  Gang  Hui  Xin  Cao  Jiayuan 《Natural Hazards》2020,104(2):1705-1722
Natural Hazards - Identification of water sources is a key issue of water inrush. This study applied a mixing model based on hydrochemical data to identify water sources and proportions. This study...  相似文献   

14.
This work constitutes the first survey of I isotope ratios for Scottish sea water including the first data for the west of Scotland. These data are of importance because of the proximity to the world’s second largest emission source of 129I to the sea, the Sellafield nuclear reprocessing plant, because of the increasing importance of the sea to land transfer of 129I and also as input data for dose estimates based on this pathway of 129I. 129I/127I ratios in SW Scotland reached 3 × 10−6 in 2004. No strong variation of I isotope ratios was found from 2003 to 2005 in Scottish sea waters. Iodine isotope ratios increased by about a factor of 6 from 1992 to 2003 in NE Scotland, in agreement with the increase of liquid 129I emissions from Sellafield over that time period. It is demonstrated that 129I/127I ratios agree better than 129I concentrations for samples from similar locations taken in very close temporal proximity, indicating that this ratio is more appropriate to interpret than the radionuclide concentration.  相似文献   

15.
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   

16.
High-purity synthetic barite powder was added to pure water or aqueous solutions of soluble salts (BaCl2, Na2SO4, NaCl and NaHCO3) at 23 ± 2 °C and atmospheric pressure. After a short pre-equilibration time (4 h) the suspensions were spiked either with 133Ba or 226Ra and reacted under constant agitation during 120-406 days. The pH values ranged from 4 to 8 and solid to liquid (S/L) ratios varied from 0.01 to 5 g/l. The uptake of the radiotracers by barite was monitored through repeated sampling of the aqueous solutions and radiometric analysis. For both 133Ba and 226Ra, our data consistently showed a continuous, slow decrease of radioactivity in the aqueous phase.Mass balance calculations indicated that the removal of 133Ba activity from aqueous solution cannot be explained by surface adsorption only, as it largely exceeded the 100% monolayer coverage limit. This result was a strong argument in favor of recrystallization (driven by a dissolution-precipitation mechanism) as the main uptake mechanism. Because complete isotopic equilibration between aqueous solution and barite was approached or even reached in some experiments, we concluded that during the reaction all or substantial fractions of the initial solid had been replaced by newly formed barite.The 133Ba data could be successfully fitted assuming constant recrystallization rates and homogeneous distribution of the tracer into the newly formed barite. An alternative model based on partial equilibrium of 133Ba with the mineral surface (without internal isotopic equilibration of the solid) could not reproduce the measured activity data, unless multistage recrystallization kinetics was assumed. Calculated recrystallization rates in the salt solutions ranged from 2.8 × 10−11 to 1.9 × 10−10 mol m−2 s−1 (2.4-16 μmol m−2 d−1), with no specific trend related to solution composition. For the suspensions prepared in pure water, significantly higher rates (∼5.7 × 10−10 mol m−2 s−1 or ∼49 μmol m−2 d−1) were determined.Radium uptake by barite was determined by monitoring the decrease of 226Ra activity in the aqueous solution with alpha spectrometry, after filtration of the suspensions and sintering. The evaluation of the Ra uptake experiments, in conjunction with the recrystallization data, consistently indicated formation of non-ideal solid solutions, with moderately high Margules parameters (WAB = 3720-6200 J/mol, a0 = 1.5-2.5). These parameters are significantly larger than an estimated value from the literature (WAB = 1240 J/mol, a0 = 0.5).In conclusion, our results confirm that radium forms solid solutions with barite at fast kinetic rates and in complete thermodynamic equilibrium with the aqueous solutions. Moreover, this study provides quantitative thermodynamic data that can be used for the calculation of radium concentration limits in environmentally relevant systems, such as radioactive waste repositories and uranium mill tailings.  相似文献   

17.
Stirred flow-through experiments were conducted for the first time with planktonic biogenic silica (BSi). We investigated the dissolution kinetics of uncleaned and chemically cleaned BSi collected in ocean surface water, sediment traps, and sediments from the Norwegian Sea, the Southern Ocean, and the Arabian Sea. The solubility at 2°C is rather constant (1000 to 1200 μM). The dissolution rates are, however, highly variable, declining with water depth, and phytoplankton reactivity is two to three orders of magnitude higher than pure siliceous oozes. The reactivity decrease correlates well with an increase in the integrated peak intensity ratios of Si-O-Si/Si-OH measured by Fourier transform infrared (FTIR) spectroscopy. The removal of organic or inorganic coatings enhance the reactivity by at least an order of magnitude. Atomic Al/Si ratios of 0.03 to 0.08 in sedimentary diatom frustules decrease significantly to 0.02 as a result of removal of inorganic coatings and detritals present. Near equilibrium, the dissolution rates exhibit a linear dependence on the degree of undersaturation. At higher degrees of undersaturation—that is, at low concentrations of dissolved silica—the dissolution rates of uncleaned samples define a nonlinear trend.The nonlinear kinetics imply that the dissolution of natural BSi is strongly accelerated in silica-depleted surface waters. The FTIR results suggest that internal condensation reactions reduce the amount of surface reaction sites and are partly responsible for the reactivity decrease with depth. The high content of Al in sedimentary BSi is likely caused by precipitation of dissolved silica with Al dissolved from minerals in sediment. Nonbiogenic silica as coatings or detritals are partly responsible for the solubility and reactivity decrease of BSi in sediments. One order of magnitude different rate constants measured in Norwegian Sea and Southern Ocean sediment trap material support the so-called opal paradox—that is, high BSi accumulation rates in sediments in spite of low BSi production rates in surface waters of the Southern Ocean.  相似文献   

18.
研究了TIMS测定铀矿石样品中234U/238U、230Th/232Th、228Ra/226Ra的方法。建立了铀矿石密闭混酸一次溶样的方法和采用阴离子、阳离子和Sr特效树脂逐级离子交换分离纯化U、Th和Ra的流程,满足了TIMS测量要求。测定结果表明:100~1000 ng的天然铀中234U/238U,其测量精密度从静态多接收的2.34%提高到动态多接收的0.47%;对230Th与232Th丰度接近、质量为1μg左右的钍,采用三带点样技术和法拉第多接收技术测定230Th/232Th,其内精度平均值为0.0048%,外精度为0.028%;采用单带加钽发射剂,ETP跳峰测定50~100 fg镭-228稀释剂中的228Ra/226Ra,其内精度小于0.10%,外精度小于0.20%。比较TIMS和HR-ICP-MS、α能谱法测定234U/238U、230Th/232Th、228Ra/226Ra结果,三者结果相吻合。TIMS测量法样品用量少、快速、准确、精密度高,是U、Th、Ra同位素比值测定方法的又一补充。  相似文献   

19.
Current designs for nuclear-waste repositories rely primarily upon subsurface geologic barriers for long-term containment. Because water and air are generally considered to be the mechanisms most likely to transport radioactivity to the surface environment, flow and transport models are important tools in repository assessment. Most models assume that the geologic medium can be treated as a continuum. A substantial body of recent work has focused on applying these models to difficult-to-solve problems, such as the simulation of variably dense or variably saturated flow and transport, large and complex flow systems, sharp solute concentration fronts, and fractured rock systems. The complex chemical interactions between the transport fluid and solid particles within the system have been analyzed using geochemical flow models, most of which assume that the system is at chemical equilibrium. The role of colloids in contaminant transport is a relatively new area of research. The large-scale effects of small-scale variability within the geologic system have been the subject of intense investigation. Inherent limitations of the continuum approach have prompted the design of models in which the flow occurs in discrete fractures. The difficulty and complexity of simulating transport has led to the development of network transport models, which represent the flow field as a series of 1-D path segments. The widespread use of models for prediction and analysis has prompted investigations of their reliability and relative merits.  相似文献   

20.
Isotopes of plutonium (Pu), cesium (Cs), and cobalt (Co) introduced into the Hudson River Estuary from fallout deposition, the erosion of fallout-contaminated surface soils, and nuclear reactor effluent (isotopes of Cs and Co only) have been measured in water column samples collected from 1975 to 1980 Isotopic measurements conducted independently by two research groups utilizing different sampling and analytical techniques have been summarized. The major conclusions drawn from the work are that for water samples collected by the two laboratories over similar time periods, the mean concentrations of nonfilterable239,240Pu (<0.45 μm) were identical at 0.13 fCi/l, mean concentrations of both137Cs and239,240Pu in suspended particulates were more divergent at 2,270±920 pCi/kg (±1 SD) and 1,430±430 pCi/kg for137Cs, and 19±8 pCi/kg and 12±4 pCi/kg for239,240Pu The behavior of239,240Pu and137Cs within the water column is shown to diverge within brackish waters Specifically, the magnitude of the137Cs distribution coefficient (K d ) can be expressed as an inverse power function of the chloride ion concentrations for chlorinities between 0.1 and 4 g Cl/l No difference in the239,240PuK d has been observed between fresh and brackish waters Based on the expected inventories of239,240Pu and137Cs within watershed soils, the current downstream transport of these radionuclides represents fractional mobilization rates on the order of 1–4 (×10−4) per year  相似文献   

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