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1.
We present a new LA–ICP–MS system for zircon fission‐track (FT) and U–Pb double dating, whereby a femtosecond laser combined with galvanometric optics simultaneously ablates multiple spots to measure average surface U contents. The U contents of zircon measured by LA–ICP–MS and standardized with the NIST SRM610 glass are comparable to those measured by the induced FT method, and have smaller analytical errors. LA–ICP–MS FT dating of seven zircon samples including three IUGS age standards is as accurate as the external detector method, but can give a higher‐precision age depending on the counting statistics of the U content measurement. Double dating of the IUGS age standards gives FT and U–Pb ages that are in agreement. A chip of the Nancy 91500 zircon has a homogeneous U content of 84 ppm, suggesting the possibility of using this zircon as a matrix‐matched U‐standard for FT dating. When using the Nancy 91500 zircon as a U‐standard, a zeta calibration value of 42–43 year cm2 for LA–ICP–MS FT dating is obtained. While this value is strictly valid only for the particular session, it can serve as a reference for other studies.  相似文献   

2.
The activities of the natural radionuclides (238U, 232Th, 226Ra and 40K) of the surface sediments in the Yangtze Estuary were determined and used to evaluate radiation hazards in the study area. The of activities of 238U, 232Th, 226Ra and 40K ranges from 14.1 to 62.3, 26.1 to 71.9, 13.7 to 52.3, and 392 to 898 Bq kg? 1, respectively, which were comparable to values of other regions in China. The activities of 232Th, 40K and 226Ra were clearly different from the global recommended values. The radium equivalent activity was less than the recommended limit of 370 Bq kg? 1; therefore, the sediment in this area can be safely used for reclamation. The external hazard index values were less than one. The average absorbed gamma dose rate and annual effective dose equivalent values were slightly greater than the world average value. 226Ra/238U and 232Th/238U ratios could potentially be applied for tracing sediment source.  相似文献   

3.
The Stavropol region of southern Russia is severely affected by human‐induced gully erosion. A lack of detailed information on the different stages of gully formation resulting from major agricultural expansion c. 100 years ago, is an obstacle for management and containment of these systems. In this study we combine measurements of particle‐bound radionuclides (137Cs, 210Pbex, 226Ra, 232Th and 40K) and classical geomorphology to investigate and reconstruct the different phases of development of a gully during the last c. 100 years. We believe the ?rst phase (1) involved an initial incision into the bottom of a small valley (catchment area c. 1 km2) about 100 years ago. A short period of rapid growth was followed by a longer stage of gully stabilization. Subsequent phases were: (2) the period 1954–1960 – re‐incision in the lower gully reach was initiated by a high‐magnitude rainfall event, and a substantial amount of sediment was delivered to the gully fan; (3) c. 1960–1986 – the knickpoint retreated slowly, sediment was redeposited nearby, and the fan surface became stable; (4) 1986–1987 – a dam was built in the gully mouth and breached shortly after construction following 2 days of high rainfall, and substantial sediment accumulated in the gully above the dam and below the spillway channel on the fan surface; (5) 1987–1993 – the knickpoint retreat continued and the lower fan surface was stable until 1993 when the last signi?cant runoff event overlayed it with c. 10 cm of fresh sediment. These detailed reconstructions of gully development stages allow the contribution of high‐magnitude events to gully growth and regional sediment delivery to be assessed. They further guide management actions to prevent such dam failures in the future. Copyright © 2004 John Wiley & Sons, Ltd.  相似文献   

4.
Radionuclides released to the environment and deposited with or onto snow can be stored over long time periods if ambient temperature stays low, particularly in glaciated areas or high alpine sites. The radionuclides will be accumulated in the snowpack during the winter unless meltwater runoff at the snow base occurs. They will be released to surface waters within short time during snowmelt in spring. In two experiments under controlled melting conditions of snow in the laboratory, radionuclide migration and runoff during melt‐freeze‐cycles were examined. The distribution of Cs‐134 and Sr‐85 tracers in homogeneous snow columns and their fractionation and potential preferential elution in the first meltwater portions were determined. Transport was associated with the percolation of meltwater at ambient temperatures above 0 °C after the snowpack became ripe. Mean migration velocities in the pack were examined for both nuclides to about 0.5 cm hr?1 after one diurnal melt‐freeze‐cycle at ambient temperatures of ?2 to 4 °C. Meltwater fluxes were calculated with a median of 1.68 cm hr?1. Highly contaminated portions of meltwater with concentration factors between 5 and 10 against initial bulk concentrations in the snowpack were released as ionic pulse with the first meltwater. Neither for caesium nor strontium preferential elution was observed. After recurrent simulated day‐night‐cycles (?2 to 4 °C), 80% of both radionuclides was released with the first 20% of snowmelt within 4 days. 50% of Cs‐134 and Sr‐85 were already set free after 24 hr. Snowmelt contained highest specific activities when the melt rate was lowest during the freeze‐cycles due to concentration processes in remaining liquids, enhanced by the melt‐freeze‐cycling. This implies for natural snowpack after significant radionuclide releases, that long‐time accumulation of radionuclides in the snow during frost periods, followed by an onset of steady meltwater runoff at low melt rates, will cause the most pronounced removal of the contaminants from the snow cover. This scenario represents the worst case of impact on water quality and radiation exposure in aquatic environments.  相似文献   

5.
Ground waters from fractured igneous and high-grade sialic metamorphic rocks frequently have elevated activity of dissolved radon (222Rn). A chemically based model is proposed whereby radium (226Ra) from the decay of uranium (238U) diffuses through the primary porosity of the rock to the water-transmitting fracture where it is sorbed on weathering products. Sorption of 226Ra on the fracture surface maintains an activity gradient in the rock matrix, ensuring a continuous supply of 226Ra to fracture surfaces. As a result of the relatively long half-life of 226Ra (1601 years), significant activity can accumulate on fracture surfaces. The proximity of this sorbed 226Ra to the active ground water flow system allows its decay progeny 222Rn to enter directly into the water. Laboratory analyses of primary porosity and diffusion coefficients of the rock matrix, radon emanation, and ion exchange at fracture surfaces are consistent with the requirements of a diffusion/ion-exchange model. A dipole-brine injection/withdrawal experiment conducted between bedrock boreholes in the high-grade metamorphic and granite rocks at the Hubbard Brook Experimental Forest, Grafton County, New Hampshire, United States (42 degrees 56'N, 71 degrees 43'W) shows a large activity of 226Ra exchanged from fracture surfaces by a magnesium brine. The 226Ra activity removed by the exchange process is 34 times greater than that of 238U activity. These observations are consistent with the diffusion/ion-exchange model. Elutriate isotopic ratios of 223Ra/226Ra and 238U/226Ra are also consistent with the proposed chemically based diffusion/ion-exchange model.  相似文献   

6.
Two expeditions (October 1989 and May 1992) were carried out to two points of the main Amazon River channel and four tributaries. The Solimões and Madeira rivers, taking their origin in the Andes, are whitewater rivers. The Negro River is a typical acid, blackwater river. The Trombetas River flows through bauxite‐rich areas, and is characterized by low concentrations of dissolved humic substances. The 238U, 234U, 232Th and 230Th activities were recorded from dissolved, suspended particulate phases and river bank sediments. The latter were analysed for their 226Ra, 228Ra and 210Pb contents, and also subjected to leaching with 0·2 M hydroxylamine–hydrochloride solution to determine the concentrations of radionuclides bound to amorphous Fe hydroxides and Mn oxides and hydroxides. The dissolved U average concentration in the Amazon system is ten times lower than the mean world river concentration. The uranium concentration observed at Óbidos in the lower Amazon (0·095 µg L?1), where the U content in the river bank sediments and suspended matter is lowest, suggests U release from the solid phase during river transport. About 485 t of U are transported annually to the Amazon delta area in dissolved form, and 1943 t bound to suspended particulate matter. Total U and Th concentrations in the river bank sediments ranged from 1·59 to 7·14 µg g?1 and from 6·74 to 32 µg g?1, respectively. The highest concentrations were observed in the Trombetas River. The proportion extracted by means of the hydroxylamine solution (HL) was relatively high for U in the Trombetas river bank sediment (31%) and for Th in the Solimões sediment (30%). According to the alpha recoil effects, the 234U/238U activity ratios of the Andean river waters and downstream Amazon water (Óbidos) were >1, but were <1 in the Negro River (at Manaus). The activity ratios of dissolved U correlate with pH and also with the U activity ratios in the river bank sediment hydroxylamine extracts. As expected, the 234U/238U activity ratios in river bank sediments were <1 in the Andean rivers and in the downstream Amazon, but they were >1 in the Trombetas and Negro rivers. Such ratios probably result from the binding of dissolved uranium to solid sediment. The 228Th/232Th ratios of river bank sediments were close to unity (except for the Negro River, where it is lower), suggesting no significant Th exchanges between the river water and the sediment. The 226Ra/232Th activity ratios were <1, and the 226Ra/228Ra activity ratios generally were significantly higher than the activity ratios of their respective parents. This perhaps is the result of easier leaching of the 226Ra parent, 230Th, from solid material (owing to the alpha recoil effect) than of the 228Ra parent. Uranium and thorium isotopes were used as tools to evaluate the chemical weathering rate of rocks in the Amazon system, which was estimated to be 2·7 cm 1000 year?1 s?1. Copyright © 2002 John Wiley & Sons, Ltd.  相似文献   

7.
Interest in preconcentration techniques for the determination of metals at ultratrace levels still continues increasingly because of some disadvantages of flameless atomic absorption spectrometry and the high costs of other sensitive methods in compared to flame atomic absorption spectrometry (FAAS). Among preconcentration techniques, solid‐phase extraction is the most popular because of a number of advantages. In this work, thiol‐containing sulfonamide resin was synthesized, characterized, and applied as a new sorption material for solid phase extraction and determination of lead in natural water samples. The optimization of experimental conditions was performed using the parameters including pH, contact time, and volumes of initial and elution solutions. After preconcentration procedure, FAAS was used for determinations. The synthesized resin exhibits the superiority in compared to the other adsorption reagents because of the fact that there is no necessity of any complexing reagent as well as high sorption capacity. Consequently, 280‐fold improvement in the sensitivity of analytical scheme was achieved by combining the slotted tube atom trap‐atomic absorption spectrometry (STAT‐FAAS) and the developed preconcentration method. The limit of detection was found to be 0.15 ng mL?1. The Pb2+ concentrations in the studied water samples were found to be in the range of 0.9–6.7 ng mL?1.  相似文献   

8.
Clement TP 《Ground water》2011,49(5):620-629
Groundwater models are routinely used in hindcasting applications to predict the past concentration levels in contaminated aquifers. These predictions are used in risk assessment and epidemiological studies, which are often completed either for resolving a court case or for developing a public‐policy solution. Hindcast groundwater modeling studies utilize a variety of computer tools with complexity levels ranging from simple analytical models to detailed three‐dimensional, multiphase, multispecies, reactive transport models. The aim of this study is to explore the value of using complex reactive transport models in hindcasting studies that have limited historic data. I review a chlorinated solvent exposure problem that occurred at a U.S. Marine Corp Base in Camp Lejeune, North Carolina and use it as an example to discuss the limits of hindcasting modeling exercises. The lessons learned from the study are used to reflect upon the following questions related to model complexity: How should we decide how much is enough? Who should decide when enough is enough?  相似文献   

9.
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10.
Here we investigate the feasibility of using alpha-spectrometric 226Ra methodology to date low U freshwater carbonate deposits (<0.1 μg g−1) by analysing Holocene freshwater travertine deposits from Esanatoglia, Umbro-Marchean Apennines, Central Italy. Previously, such methods have been tested on hydrothermal deposits, which are characterised by high Ra and U. We calculate a 226Ra age estimate of 2.9±0.4 ka (1σ) for Holocene travertine that is in reasonable agreement with archaeological evidence by assuming that the 226Ra initial activity of the Holocene travertine is comparable with that of present-day carbonate deposits in the same area. We also investigate the use of Ba to normalise 226Ra activities. Comparison of age estimates based on Ra methods with ages derived from alpha-spectrometric 230Th/234U isochron techniques for the same co-eval sub-samples indicates that, where only alpha-spectrometric methods are available, the former are likely to be much more useful for Holocene travertine material, especially if there is a significant detrital component.  相似文献   

11.
A fiber extraction technique is used to concentrate Ra and Th isotopes from 1000 liters or more of seawater. Natural226Ra and234Th are used as yield tracers. In the equatorial Pacific the228Ra activity of surface water varies from 20 to 1 dpm/1000 kg and generally decreases away from continental shelf areas. Across the Peru Current System, this decrease is modeled as one-dimensional diffusion and indicates the possibility of two flow regimes with distinct characteristic mixing lengths and apparent eddy diffusivities of 105 and 107 cm2/s. The perturbing effects of advection and equatorial upwelling west of the Galapagos Islands are noted. Off the coast of Southern California a vertical228Ra distribution gives an apparent diffusivity of 1.6 cm2/s for the upper thermocline.226Ra concentrations near the coast appear to be higher than the open ocean values at comparable depths, which may reflect supply of this isotope from continental shelf sediments and/or upwelling. The insoluble daughter/soluble parent activity ratios228Th/228Ra and234Th/238U in the equatorial Pacific surface water display latitudinal trends which may be correlated with productivity variations. Near the coast of California these ratios reflect the differing oceanographic conditions north and south of Pt. Conception indicating a mean chemical removal time constant on the order of 4 months for Th and other highly reactive elements within the Southern California Bight. The232Th content of seawater sampled is less than 0.1 μg/1000 1; most of the published values for seawater232Th could well be too high. A comparison of the two methods of determining228Ra (via228Ac and via228Th) made on 64 seawater samples shows that the time delay required by the228Th method is more than compensated by its better analytical simplicity and precision.  相似文献   

12.
In this study, the practical methodologies are described for the determination of the factors for the self-absorption effect (Fs), spectral interferences (Fcsi), and true coincidence summing effects (Fcoi), which are used in direct gamma-spectrometric measurement of radionuclides such as 210Pb, 238U, 234Th, 226Ra, 214Pb, 228Ac, 208Tl, 214Bi, 137Cs and 40K in samples. To validate the applied methods, certified reference materials (CRMs) of lake and stream sediments were measured with an n-type Germanium (Ge) detector-calibrated using a multinuclide reference source. The highest self-absorption correction factors ranged from Fs = 1.44–2.10 for 46.5 keV peak (210Pb) and Fs = 1.25–1.60 for 63.3 keV peak (234Th) lying in the low energy region of the spectrum. The systematic influence was observed for 186.2 keV (226Ra) peak due to spectral interferences with the 235U contribution. For this peak, Fcsi is changed from 0.921 to 0.955. Additionally, the present study suggests that true coincidence summing (TCS) effects are not dominant, except for 208Tl and 214Bi for which Fcoi ranged from 1.179 to 1.192 an ranged from 1.140 to 1.151, respectively.  相似文献   

13.
The concentrations of radionuclides of the U-Th series (238U,234Th,234U,230Th,226Ra,210Pb,210Po, and232Th,228Ra,228Th) in the water of Narragansett Bay are reported. Analysis of the total, particulate, dissolved and colloidal forms of Th isotopes reveal a consistent removal behavior which is controlled mainly by the particulate matter concentration and the sediment resuspension rate. Half-removal times of Th from solution onto particles range from 1.5 to 15 days, and settling velocities of Th containing particles range generally between 1 and 11 m/day.210Pb and210Po concentrations are seasonally dependent, with higher concentrations and slower removal during the early summer (half-removal times from solution onto particles of 1–5 days in winter and up to 2 months in early summer).  相似文献   

14.
Time‐lapse refraction can provide complementary seismic solutions for monitoring subtle subsurface changes that are challenging for conventional P‐wave reflection methods. The utilization of refraction time lapse has lagged behind in the past partly due to the lack of robust techniques that allow extracting easy‐to‐interpret reservoir information. However, with the recent emergence of the full‐waveform inversion technique as a more standard tool, we find it to be a promising platform for incorporating head waves and diving waves into the time‐lapse framework. Here we investigate the sensitivity of 2D acoustic, time‐domain, full‐waveform inversion for monitoring a shallow, weak velocity change (?30 m/s, or ?1.6%). The sensitivity tests are designed to address questions related to the feasibility and accuracy of full‐waveform inversion results for monitoring the field case of an underground gas blowout that occurred in the North Sea. The blowout caused the gas to migrate both vertically and horizontally into several shallow sand layers. Some of the shallow gas anomalies were not clearly detected by conventional 4D reflection methods (i.e., time shifts and amplitude difference) due to low 4D signal‐to‐noise ratio and weak velocity change. On the other hand, full‐waveform inversion sensitivity analysis showed that it is possible to detect the weak velocity change with the non‐optimal seismic input. Detectability was qualitative with variable degrees of accuracy depending on different inversion parameters. We inverted, the real 2D seismic data from the North Sea with a greater emphasis on refracted and diving waves’ energy (i.e., most of the reflected energy was removed for the shallow zone of interest after removing traces with offset less than 300 m). The full‐waveform inversion results provided more superior detectability compared with the conventional 4D stacked reflection difference method for a weak shallow gas anomaly (320 m deep).  相似文献   

15.
The energy released in a spontaneous decay process of natural radionuclides is the main source of the total radiation dose to human beings. Natural radionuclides are widely distributed in soil, rocks, air, and groundwater. In present investigation, the analysis of terrestrial radionuclides such as 226Ra, 232Th, and 40K in soil and sand of Chattarpur area of southeastern coast of Odisha has been carried out using NaI(Tl) gamma ray detector. The higher activity concentrations of naturally occurring radionuclides have been reported from the study area. The gamma radiationdose originating from the terrestrial radionuclides was found to vary from 95 to 1813 nGy/h with an average of 700 nGy/h. This study is important to generate a baseline data of radiation exposure in the area. Health hazard effects due to natural radiation exposure are discussed in details.  相似文献   

16.
The natural radioactivity due to radium, thorium, and potassium in building material samples contribute to the radiation dose received by human beings significantly. It is essential to evaluate the activity levels of these nuclides for the assessment of natural radiation dose. Activity concentrations of the gamma emitting primordial radionuclides 232Th, 226Ra, and 40K were measured using high resolution gamma spectrometry technique with high purity germanium (HPGe) detector in building materials: sand, brick, granite, cement and rock, collected from various areas of Gulbarga and Koppal districts. The standard ASTM procedure was followed for the sample preparation. The distribution of radionuclides and variation in activity concentration depend upon the rock formation and the geological properties of the region. The activity of the three radionuclides, 232Th, 226Ra, and 40K, were found to be in the range of 3.1–227.1, 1.6–111, and 23.2–1505 Bq/kg, respectively. The dose related radiological parameters were also calculated for all the samples and the observations show that the activity concentrations of the radionuclides are well within the UNSCEAR limits.  相似文献   

17.
Many studies indicate that small‐scale heterogeneity and/or mobile–immobile mass exchange produce transient non‐Fickian plume behavior that is not well captured by the use of the standard, deterministic advection‐dispersion equation (ADE). An extended ADE modeling framework is presented here that is based on continuous time random walk theory. It can be used to characterize non‐Fickian transport coupled with simultaneous sequential first‐order reactions (e.g., biodegradation or radioactive decay) for multiple degrading contaminants such as chlorinated solvents, royal demolition explosive, pesticides, and radionuclides. To demonstrate this modeling framework, new transient analytical solutions are derived and are inverted in Laplace space. Closed‐form, steady‐state, multi‐species analytical solutions are also derived for non‐Fickian transport in highly heterogeneous aquifers with linear sorption–desorption and matrix diffusion for use in spreadsheets. The solutions are general enough to allow different degradation rates for the mobile and immobile zones. The transient solutions for multi‐species transport are applied to examine the effects of source remediation on the natural attenuation of downgradient plumes of both parent and degradation products in highly heterogeneous aquifers. Results for representative settings show that the use of the standard, deterministic ADE can over‐estimate cleanup rates and under‐predict the cleanup timeframe in comparison to the extended ADE analytical model. The modeling framework and calculations introduced here are also applied for a 30 year groundwater cleanup program at a site in Palm Bay, Florida. The simulated plume concentrations using the extended ADE exhibited agreement with observed long concentration tails of trichloroethene, cis 1,2 DCE, and VC that remained above cleanup goals.  相似文献   

18.
We assess the relative merits of application of the most commonly used field methods (soil‐water balance (SWB), chloride mass balance (CMB) and soil moisture monitoring (NP)) to determine recharge rates in micro‐irrigated and non‐irrigated areas of a semi‐arid coastal orchard located in a relatively complex geological environment. Application of the CMB method to estimate recharge rates was difficult owing to the unusually high, variable soil‐water chloride concentrations. In addition, contrary to that expected, the chloride concentration distribution at depths below the root zone in the non‐irrigated soil profiles was greater than that in the irrigated profiles. The CMB method severely underestimated recharge rates in the non‐irrigated areas when compared with the other methods, although the CMB method estimated recharge rates for the irrigated areas, that were similar to those from the other methods, ranging from 42 to 141 mm/year. The SWB method, constructed for a 15‐year period, provided insight into the recharge process being driven by winter rains rather than summer irrigation and indicated an average rate of 75 mm/year and 164 mm/year for the 1984 – 98 and 1996 – 98 periods, respectively. Assuming similar soil‐water holding capacity, these recharge rates applied to both irrigated and non‐irrigated areas. Use of the long period of record was important because it encompassed both drought and heavy rainfall years. Successful application of the SWB method, however, required considerable additional field measurements of orchard ETc, soil‐water holding capacity and estimation of rainfall interception – runoff losses. Continuous soil moisture monitoring (NP) was necessary to identify both daily and seasonal seepage processes to corroborate the other recharge estimates. Measured recharge rates during the 1996 – 1998 period in both the orchards and non‐irrigated site averaged 180 mm/year. The pattern of soil profile drying during the summer irrigation season, followed by progressive wetting during the winter rainy season was observed in both irrigated and non‐irrigated soil profiles, confirming that groundwater recharge was rainfall driven and that micro‐irrigation did not ‘predispose’ the soil profile to excess rainfall recharge. The ability to make this recharge assessment, however, depended on making multiple field measurements associated with all three methods, suggesting that any one should not be used alone. Copyright © 2000 John Wiley & Sons, Ltd.  相似文献   

19.
The Future Midwestern Landscapes (FML) project is part of the U.S. Environmental Protection Agency's Ecosystem Services Research Program. The goal of the FML project is to quantify changes in ecosystem services across the Midwestern region as a result of the growing demand for biofuels. Watershed models are an efficient way to quantify ecosystem services of water quality and quantity. By calibrating models, we can better capture watershed characteristics before they are applied to make predictions. The Kaskaskia River watershed in Illinois was selected to investigate the effectiveness of different calibration strategies (single‐site and multi‐site calibrations) for streamflow, total suspended sediment (TSS) and total nitrogen (TN) loadings using the Soil and Water Assessment Tool. Four USGS gauges were evaluated in this study. Single‐site calibration was performed from a downstream site to an upstream site, and multi‐site calibration was performed and fine‐tuned based on the single‐site calibration results. Generally, simulated streamflow and TSS were not much affected by different calibration strategies. However, when single‐site calibration was performed at the most downstream site, the Nash–Sutcliffe efficiency (NSE) values for TN ranged between ?0.09 and 0.53 at the other sites; and when single‐site calibration was performed at the most upstream site, the NSE values ranged between ?8.38 and ?0.07 for the other sites. The NSE values for TN were improved to 0.5 – 0.59 for all four sites when multi‐site calibration was performed. The results of the multi‐site calibration and validation showed an improvement on model performance on TN and highlighted that multi‐site calibrations are needed to assess the hydrological and water quality processes at various spatial scales. Copyright © 2012 John Wiley & Sons, Ltd.  相似文献   

20.
The value of studying artificially-produced radionuclides in the marine environment is discussed in the wider context of monitoring sediments for other metal pollutants. Differences in the dispersion of selected radionuclides discharged from the same known source are used to illustrate the sort of changes in phase or speciation which must occur with other metal pollutants, but which cannot be demonstrated directly because of the multiplicity of sources. Various chemical and physical procedures are discussed which can be applied to a study of heavy metal associations with marine sediments, as are questions such as the existence, or otherwise, of mechanisms for the slow release of adsorbed material from the buried sediment back into the water column. Suggestions are made as to how radionuclide studies may be helpful in answering questions such as these, which are considered to be vital for the meaningful interpretation of sediment analyses.  相似文献   

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