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1.
To investigate the possible variations of Rn concentration in crystalline rocks as a function of flow conditions, a field study was carried out of a fractured aquifer in granite. The method is based on the in situ measurement of Rn in groundwater, aquifer tests for the determination of hydraulic characteristics of the aquifer and laboratory measurement of Rn exhalation rate from rocks. A simple crack model that simulates the Rn concentration in waters circulating in a fracture intersecting a borehole was also tested. The Rn concentrations in groundwaters from boreholes of the study site ranged from 192 to 1597 Bq L−1. The Rn exhalation rates of selected samples of granite and micaschist were determined from laboratory experiments. The results yielded fluxes varying from 0.5 to 1.3 mBq m−2 s−1 in granite and from 0.5 to 0.9 mBq m−2 s−1 in micaschists. Pumping tests were performed in the studied boreholes to estimate the transmissivity and calculate the equivalent hydraulic aperture of the fractures. Transmissivities ranged from 10−5 to 10−3 m2 s−1. Using the cubic law, hydraulic equivalent fracture apertures were calculated to be in the range of 0.5–2.3 mm.  相似文献   

2.
The recommended concentrations of 239Pu, 240Pu and 239+240Pu in reference material IAEA‐315 (marine sediment) were estimated by three analytical methods: isotope dilution thermal ionisation mass spectrometry (TIMS), isotope dilution inductively coupled plasma‐mass spectrometry (ICP‐MS) and alpha spectrometry. The determination of 239Pu and 240Pu (239+240Pu by alpha spectrometry) was carried out with samples from randomly selected bottles using each method. Plutonium‐238 was also measured by alpha spectrometry. A plutonium‐242 reference material was used as a spike for the quantitative analysis. The influence of 242Pu in the samples was therefore calculated; however, this contribution was less than the range of uncertainty and did not influence the final results. The obtained data were statistically analysed using variance component analysis and paired comparison. The combined standard uncertainties from “method/measurement”, “bottle” and “sub‐sample” were in the order of 3 to 6%. The main contributions to the uncertainty were from the material heterogeneity and from systematic differences between methods. Based on this study with twenty‐seven analyses using 10–14 g sample mass, concentrations of (38 ± 3) Bq kg?1, (28 ± 3) Bq kg?1 and (66 ± 4) Bq kg?1 are proposed as recommended values for 239Pu, 240Pu and 239+240Pu, respectively, and (9.5 ± 0.4) Bq kg?1 for 238Pu as an information value in reference material IAEA‐315. In mass concentration units, these amount to (16.4 ± 1.2) ng kg?1, (3.3 ± 0.4) ng kg?1 and (0.015 ± 0.003) ng kg?1 for 239Pu, 240Pu and 238Pu, respectively. The certified reference materials NIST 4350B and NIST 4354 were also analysed by TIMS for quality assurance of the method used in this study.  相似文献   

3.
The Pu isotopes, 239Pu and 240Pu, were determined in annually-banded skeletons of an accurately dated (1943-1999) modern coral (Porites lobata) from Guam Island to identify historical Pu sources to the tropical Northwest Pacific Ocean. Activity concentrations of 239+240Pu and 240Pu/239Pu atom ratios were determined in the dated coral bands using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands and global fallout were identified as the two main sources. The Guam site was dominated by PPG close-in fallout in the 1950s, with an average 240Pu/239Pu atom ratio of 0.315 ± 0.005. In addition, a higher 240Pu/239Pu atom ratio (0.456 ± 0.020) was observed that could be attributed to fallout from the “Ivy Mike” thermonuclear detonation in 1952. The atom ratio decreased in the 1960s and 1970s due to increase in the global fallout with a low 240Pu/239Pu atom ratio (∼0.18). Recent coral bands (1981-1999) are dominated by the transport of remobilised Pu, with high 240Pu/239Pu atom ratios, from the Marshall Islands to Guam Island along the North Equatorial Current (NEC). This remobilised Pu was estimated to comprise 69% of the total Pu in the recent coral bands, although its contribution was variable over time.  相似文献   

4.
To advance understanding of hydrological influences on As concentrations within groundwaters of Southeast Asia, the flow system of an As-rich aquifer on the Mekong Delta in Cambodia where flow patterns have not been disturbed by irrigation well pumping was examined. Monitoring of water levels in a network of installed wells, extending over a 50 km2 area, indicates that groundwater flow is dominated by seasonally-variable gradients developed between the river and the inland wetland basins. While the gradient inverts annually, net groundwater flow is from the wetlands to the river. Hydraulic parameters of the aquifer (K ≈ 10−4 ms−1) and overlying clay aquitard (K ≈ 10−8 ms−1) were determined using grain size, permeameter and slug test analyses; when coupled with observed gradients, they indicate a net groundwater flow velocity of 0.04–0.4 ma−1 downward through the clay and 1–13 ma−1 horizontally within the sand aquifer, producing aquifer residence times on the order 100–1000 a. The results of numerical modeling support this conceptual model of the flow system and, when integrated with observed spatial trends in dissolved As concentrations, reveal that the shallow sediments (upper 2–10 m of fine-grained material) are an important source of As to the underlying aquifer.  相似文献   

5.
Iodine-129 and 238Pu, 239Pu and 240Pu are radionuclides posing a long-term safety concern due to their potential integration in bio and geo-chemical cycles and their significant half-lives. They are present throughout the environment at very low levels, and more particularly, nuclear fuel reprocessing plants (NRP) have been identified as local sources of these radionuclides. However, due to measurement difficulties, published data concerning their activity levels in terrestrial environments around NRP facilities remain scarce. The aim of the present paper is to communicate 129I, 238Pu and 239+240Pu measurements results from the area surrounding the Marcoule NRP, which is situated in SE France. Several vegetation samples were collected around the nuclear installation in 1999 and 2000, in order to examine the possible impacts of its atmospheric I and Pu discharges. Based on 238Pu/239+240Pu activity ratios and 129I/127I isotopic ratios, local increases in Pu and 129I were detected and related to industrial activity.  相似文献   

6.
This paper presents a detailed survey of the activities of selected man-made radionuclides in peat deposits located in SW Spitsbergen. Peat cores from the High Arctic (SW Spitsbergen) were analyzed by gamma spectrometry (137Cs), alpha spectrometry (238Pu, 239,240Pu, 241Am activities) and by ICPMS (240Pu/239Pu atom ratios). Maximum activities evident in the peats correspond to the 1963/1964 global maximum fallout from atmospheric testing of nuclear weapons; some of the activity profiles have been altered post-deposition by water infiltration. Activity ratios of 238Pu/239+240Pu, 241Am/239+240Pu, 239+240Pu/137Cs and 240Pu/239Pu atom ratios indicate mixing between global (stratospheric) and regional (tropospheric) sources of these radionuclides in the Svalbard area. The 238Pu/239+240Pu activity ratios varied from 0.02 ± 0.01 to 0.09 ± 0.03, suggesting global fallout as the dominant source of Pu. The 239+240Pu/137Cs activity ratios varied from 0.01 ± 0.01 to 0.42 ± 0.11, which apparently arises from the post-depositional mobility of 137Cs. The 241Am/239+240Pu activity ratios ranged between 0.10 ± 0.02 and 1.5 ± 0.3 and exceed the published global fallout ratio for Svalbard of 0.37 due to the relatively higher geochemical mobility of Pu vs. Am and/or ingrowth of Am from the decay of 241Pu. The atom ratio 240Pu/239Pu ranged from 0.142 ± 0.006 to 0.241 ± 0.027; however, the vast majority of peat samples exhibited 240Pu/239Pu atom ratios similar to the stratospheric fallout (∼0.18).  相似文献   

7.
Doklady Earth Sciences - The contents of isotopes of plutonium (238Pu and 239, 240Pu) and 137Cs in samples of bottom sediments and hydrobionts (water moss, amphipods, and caddisfly larvae with...  相似文献   

8.
The radionuclide burden of vegetation comprising a tide-washed pasture at Ince Marsh in the Mersey Estuary, U.K., derives mainly from adhered external particulates originating as suspended sediments in estuarine water. Radionuclide concentrations are dominated by the growth cycle of the vegetation, with the highest winter levels of contamination activity an order of magnitude greater than the lowest levels in mid-summer. A secondary effect due to sediment transfer during periods of severe flooding produces subsidiary features on this dominant seasonal profile. Radionuclide concentrations on vegetation are in the range137Cs=8–191,134Cs=0.3–0.9,241Am=0.6–46,238Pu=0.1–1.5, and239/240Pu=0.8–44 Bq kg−1. These ranges reflect the relative concentrations of radionuclides in estuarine sediment (137Cs=615,241Am=202, and239/240Pu=104 Bq kg−1) rather than the values in filtered estuary water (137Cs=0.4,241Am=0.001, and239/240Pu=0.001 Bq 1−1). Median Kd values for these radionuclide species are Cs=1,400, Am=200,000, and Pu=80,000 1 kg−1).  相似文献   

9.
The shallow aquifer beneath the Western Snake River Plain (Idaho, USA) exhibits widespread elevated arsenic concentrations (up to 120 μg L−1). While semi-arid, crop irrigation has increased annual recharge to the aquifer from approximately 1 cm prior to a current rate of >50 cm year−1. The highest aqueous arsenic concentrations are found in proximity to the water table (all values >50 μg L−1 within 50 m) and concentrations decline with depth. Despite strong vertical redox stratification within the aquifer, spatial distribution of aqueous species indicates that redox processes are not primary drivers of arsenic mobilization. Arsenic release and transport occur under oxidizing conditions; groundwater wells containing dissolved arsenic at >50 μg L−1 exhibit elevated concentrations of O2 (average 4 mg L−1) and NO3 (average 8 mg L−1) and low concentrations of dissolved Fe (<20 μg L−1). Sequential extractions and spectroscopic analysis of surficial soils and sediments indicate solid phase arsenic is primarily arsenate and is present at elevated concentrations (4–45 mg kg−1, average: 17 mg kg−1) relative to global sedimentary abundances. The highest concentrations of easily mobilized arsenic (up to 7 mg kg−1) are associated with surficial soils and sediments visibly stained with iron oxides. Batch leaching experiments on these materials using irrigation waters produce pore water arsenic concentrations approximating those observed in the shallow aquifer (up to 152 μg L−1). While As:Cl aqueous phase relationships suggest minor evaporative enrichment, this appears to be a relic of the pre-irrigation environment. Collectively, these data indicate that infiltrating irrigation waters leach arsenic from surficial sediments to the underlying aquifer.  相似文献   

10.
Sediments from the Aquia aquifer in coastal Maryland were collected as part of a larger study of As in the Aquia groundwater flow system where As concentration are reported to reach levels as high as 1072 nmol kg−1, (i.e., ∼80 μg/L). To test whether As release is microbially mediated by reductive dissolution of Fe(III) oxides/oxyhydroxides within the aquifer sediments, the Aquia aquifer sediment samples were employed in a series of microcosm experiments. The microcosm experiments consisted of sterilized serum bottles prepared with aquifer sediments and sterilized (i.e., autoclaved), artificial groundwater using four experimental conditions and one control condition. The four experimental conditions included the following scenarios: (1) aerobic; (2) anaerobic; (3) anaerobic + acetate; and (4) anaerobic + acetate + AQDS (anthraquinone-2,6-disulfonic acid). AQDS acts as an electron shuttle. The control condition contained sterilized aquifer sediments kept under anaerobic conditions with an addition of AQDS. Over the course of the 27 day microcosm experiments, dissolved As in the unamended (aerobic and anaerobic) microcosms remained constant at around ∼28 nmol kg−1 (2 μg/L). With the addition of acetate, the amount of As released to the solution approximately doubled reaching ∼51 nmol kg−1 (3.8 μg/L). For microcosm experiments amended with acetate and AQDS, the dissolved As concentrations exceeded 75 nmol kg−1 (5.6 μg/L). The As concentrations in the acetate and acetate + AQDS amended microcosms are of similar orders of magnitude to As concentrations in groundwaters from the aquifer sediment sampling site (127-170 nmol kg−1). Arsenic concentrations in the sterilized control experiments were generally less than 15 nmol kg−1 (1.1 μg/L), which is interpreted to be the amount of As released from Aquia aquifer sediments owing to abiotic, surface exchange processes. Iron concentrations released to solution in each of the microcosm experiments were higher and more variable than the As concentrations, but generally exhibited similar trends to the As concentrations. Specifically, the acetate and acetate + AQDS amended microcosm typically exhibited the highest Fe concentrations (up to 1725 and 6566 nmol kg−1, respectively). The increase in both As and Fe in the artificial groundwater solutions in these amended microcosm experiments strongly suggests that microbes within the Aquia aquifer sediments mobilize As from the sediment substrate to the groundwaters via Fe(III) reduction.  相似文献   

11.
Sixty five urban road dust samples were collected from different land use areas of ∼240 km2 in Xi’an, China. The concentrations of Ag, As, Cr, Cu, Hg, Pb, Sb and Zn were determined to investigate potentially harmful element (PHE) contamination, distribution and possible sources. In addition, the concentrations in different size fractions were measured to assess their potential impact on human health. The highest concentrations were found in the fraction with particle diameters between 80 μm and 101 μm, the finest particles (<63 μm) were not the most important carriers for Ag, As, Cd, Cr, Cu, Hg, Pb and Zn. The percentages of these elements in particles with diameters less than 63 μm (PM63) and less than 101 μm (PM101) were in the range of 7–15%, and 30–55%, respectively. Three main factors influencing element distributions have been identified: (a) industrial activities; (b) prior agricultural land use; and (c) other activities commonly found in urban areas, such as traffic, coal combustion, waste dumping, and building construction/renovation. The highest concentrations were found in industrial areas for As (20 mg kg−1), Cr (853 mg kg−1), Cu (1071 mg kg−1), Pb (3060 mg kg−1) and Zn (2112 mg kg−1), and in previous agricultural areas for Ag and Hg, indicating significant contributions from industrial activities and prior agricultural activities.  相似文献   

12.
To study the geological control on groundwater As concentrations in Red River delta, depth-specific groundwater sampling and geophysical logging in 11 monitoring wells was conducted along a 45 km transect across the southern and central part of the delta, and the literature on the Red River delta’s Quaternary geological development was reviewed. The water samples (n = 30) were analyzed for As, major ions, Fe2+, H2S, NH4, CH4, δ18O and δD, and the geophysical log suite included natural gamma-ray, formation and fluid electrical conductivity. The SW part of the transect intersects deposits of grey estuarine clays and deltaic sands in a 15–20 km wide and 50–60 m deep Holocene incised valley. The NE part of the transect consists of 60–120 m of Pleistocene yellowish alluvial deposits underneath 10–30 m of estuarine clay overlain by a 10–20 m veneer of Holocene sediments. The distribution of δ18O-values (range −12.2‰ to −6.3‰) and hydraulic head in the sample wells indicate that the estuarine clay units divide the flow system into an upper Holocene aquifer and a lower Pleistocene aquifer. The groundwater samples were all anoxic, and contained Fe2+ (0.03–2.0 mM), Mn (0.7–320 μM), SO4 (<2.1 μM–0.75 mM), H2S (<0.1–7.0 μM), NH4 (0.03–4.4 mM), and CH4 (0.08–14.5 mM). Generally, higher concentrations of NH4 and CH4 and low concentrations of SO4 were found in the SW part of the transect, dominated by Holocene deposits, while the opposite was the case for the NE part of the transect. The distribution of the groundwater As concentration (<0.013–11.7 μM; median 0.12 μM (9 μg/L)) is related to the distribution of NH4, CH4 and SO4. Low concentrations of As (?0.32 μM) were found in the Pleistocene aquifer, while the highest As concentrations were found in the Holocene aquifer. PHREEQC-2 speciation calculations indicated that Fe2+ and H2S concentrations are controlled by equilibrium for disordered mackinawite and precipitation of siderite. An elevated groundwater salinity (Cl range 0.19–65.1 mM) was observed in both aquifers, and dominated in the deep aquifer. A negative correlation between aqueous As and an estimate of reduced SO4 was observed, indicating that Fe sulphide precipitation poses a secondary control on the groundwater As concentration.  相似文献   

13.
Strontium-90 is a beta emitting radionuclide produced during nuclear fission, and is a problem contaminant at many nuclear facilities. Transport of 90Sr in groundwaters is primarily controlled by sorption reactions with aquifer sediments. The extent of sorption is controlled by the geochemistry of the groundwater and sediment mineralogy. Here, batch sorption experiments were used to examine the sorption behaviour of 90Sr in sediment–water systems representative of the UK Sellafield nuclear site based on groundwater and contaminant fluid compositions. In experiments with low ionic strength groundwaters (<0.01 mol L−1), pH variation is the main control on sorption. The sorption edge for 90Sr was observed between pH 4 and 6 with maximum sorption occurring (Kd ∼ 103 L kg−1) at pH 6–8. At ionic strengths above 10 mmol L−1, and at pH values between 6 and 8, cation exchange processes reduced 90Sr uptake to the sediment. This exchange process explains the lower 90Sr sorption (Kd ∼ 40 L kg−1) in the presence of artificial Magnox tank liquor (IS = 29 mmol L−1). Strontium K-edge EXAFS spectra collected from sediments incubated with Sr2+ in either HCO3-buffered groundwater or artificial Magnox tank liquor, revealed a coordination environment of ∼9 O atoms at 2.58–2.61 Å after 10 days. This is equivalent to the Sr2+ hydration sphere for the aqueous ion and indicates that Sr occurs primarily in outer sphere sorption complexes. No change was observed in the Sr sorption environment with EXAFS analysis after 365 days incubation. Sequential extractions performed on sediments after 365 days also found that ∼80% of solid associated 90Sr was exchangeable with 1 M MgCl2 in all experiments. These results suggest that over long periods, 90Sr in contaminated sediments will remain primarily in weakly bound surface complexes. Therefore, if groundwater ionic strength increases (e.g. by saline intrusion related to sea level rise or by design during site remediation) then substantial remobilisation of 90Sr is to be expected.  相似文献   

14.
We present some of the first analyses of the stable isotopic composition of dissolved silicon (Si) in groundwater. The groundwater samples were from the Navajo Sandstone aquifer at Black Mesa, Arizona, USA, and the Si isotope composition of detrital feldspars and secondary clay coatings in the aquifer were also analyzed. Silicon isotope compositions were measured using high-resolution multi-collector inductively coupled mass spectrometry (HR-MC-ICP-MS) (Nu1700 & NuPlasma HR). The quartz dominated bulk rock and feldspar separates have similar δ30Si of −0.09 ± 0.04‰ and −0.15 ± 0.04‰ (±95% SEM), respectively, and clay separates are isotopically lighter by up to 0.4‰ compared to the feldspars. From isotopic mass-balance considerations, co-existing aqueous fluids should have δ30Si values heavier than the primary silicates. Positive δ30Si values were only found in the shallow aquifer, where Si isotopes are most likely fractionated during the dissolution of feldspars and subsequent formation of clay minerals. However, δ30Si decreases along the flow path from 0.56‰ to −1.42‰, representing the most negative dissolved Si isotope composition so far found for natural waters. We speculate that the enrichment in 28Si is due to dissolution of partly secondary clay minerals and low-temperature silcretes in the Navajo Sandstone. The discovery of the large range and systematic shifts of δ30Si values along a groundwater flow path illustrates the potential utility of stable Si isotopes for deciphering the Si cycling in sedimentary basins, tracing fluid flow, and evaluating global Si cycle.  相似文献   

15.
The present study demonstrates the importance of hydrogeochemical characteristics (groundwater flow and recharge) of an aquifer in the release of As to groundwater. The study area (∼20 km2) is located in Chakdaha block, Nadia district, West Bengal, which hosts groundwaters of variable As content. The spatial distribution pattern of As is patchy with areas containing groundwater that is high in As (>200 μg L−1) found in close vicinity to low As (<50 μg L−1) groundwaters (within 100 m). The concentration of groundwater As is found to decrease with depth. In addition, the data shows that there is no conspicuous relationship between high groundwater As concentration and high groundwater abstraction, although the central cone of depression has enlarged over 2 a and is extending towards the SE of the study area. The river Hooghly, which forms the NW boundary of the study site, shows dual behaviour (effluent and influent during pre- and post-monsoon periods, respectively), complicating the site hydrogeology. The observed groundwater flow lines tend to be deflected away from the high As portion of the aquifer, indicating that groundwater movement is very sluggish in the As-rich area. This leads to a high residence time for this groundwater package, prolonging sediment–water interaction, and hence facilitating groundwater As release.  相似文献   

16.
The Xunyang Hg mine (XMM) situated in Shaanxi Province is an active Hg mine in China. Gaseous elemental Hg (GEM) concentrations in ambient air were determined to evaluate its distribution pattern as a consequence of the active mining and retorting in the region. Total Hg (HgT) and methylmercury (MeHg) concentrations in riparian soil, sediment and rice grain samples (polished) as well as Hg speciation in surface water samples were measured to show local dispersion of Hg contamination. As expected, elevated concentrations of GEM were found, ranging from 7.4 to 410 ng m−3. High concentrations of HgT and MeHg were also obtained in riparian soils, ranged from 5.4 to 120 mg kg−1 and 1.2 to 11 μg kg−1, respectively. Concentrations of HgT and MeHg in sediment samples varied widely from 0.048 to 1600 mg kg−1 and 1.0 to 39 μg kg−1, respectively. Surface water samples showed elevated HgT concentrations, ranging from 6.2 to 23,500 ng L−1, but low MeHg concentrations, ranging from 0.022 to 3.7 ng L−1. Rice samples exhibited high concentrations of 50–200 μg kg−1 in HgT and of 8.2–80 μg kg−1 in MeHg. The spatial distribution patterns of Hg speciation in the local environmental compartments suggest that the XMM is the source of Hg contaminations in the study area.  相似文献   

17.
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18.
Researchers of the Vernadsky Institute of Geochemistry and Analytical Chemistry of the Russian Academy of Sciences created a luminescence photometer of a new generation for the determination of trace amounts of uranium and transuranium elements (TUE). The limits of detection for actinides vary from 0.3 pg for uranium and neptunium to 2.0 pg for plutonium. For 237Np, the relative limit of detection is 0.008 Bq/L. The photometer was tested in the radioecological monitoring of a number of polluted zones in Russia. The dynamics of actinide migration in all of the studied zones enhanced in the series 239Pu < 241Am < 237Np. In this series, concentrations of radionuclides in water-soluble and exchange forms that are most mobile and determine the migration mobility of chemical elements increased in all of the studied soil types. In the group of fulvic acids, concentrations of radionuclides decreased in the series 237Np > 241Am > 239Pu irrespectively of the soil. In the group of humic acids, concentrations of radionuclides increased in the series 237Np < 239Pu < 241Am. The sorption coefficients of radionuclides by bottom sediments of the Markha River (Kraton-3 underground nuclear explosion site) and Lake Kyzyltash (East Urals Radioactive Trace) were calculated. Bioaccumulation factors of radionuclides by different plants in the impact area of the Kraton underground nuclear explosion were determined depending on the plant type.  相似文献   

19.
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   

20.
The concentrations of 238Pu, 239 + 240Pu, 241Am and 137Cs were determined in rain samples collected at Monaco in the course of 1978–1979. Based on these data, the annual deliveries of these radionuclides to the Mediterranean by rain are computed to be 0.18 ± 0.01 pCim?2 for 238Pu, 8.1 ± 0.1 pCim?2 for 239 + 240Pu, 0.58 ± 0.02 pCim?2 for 241Am and 351 ± 4 pCim?2 for 137Cs.Comparing the delivery data with the mixed layer inventories of 239 + 240Pu and 241Am in the Mediterranean, the upper limits of the mean residence time of these radionuclides in the mixed layer were estimated to be 12.3 yr for 239 + 240pu and 2.9 yr for 241Am. These values are consistent with the conclusion deduced from the vertical distribution pattern of these transuranic elements in the Mediterranean.Based on delivery values, the annual activity ratios for 238pu239 + 240Pu, 241Am239 + 240Pu and 239 + 240pu137Cs are found to be 0,022, 0.072 and 0.023 respectively. The 238pu239 + 240pu and 239 + 240Pu137Cs activity ratios vary within relatively narrow ranges with time, while a much wider variation was observed for the 241Am239 + 240Pu activity ratio. The cause of the wider variation of the 241Am239 + 240Pu ratio may be related to the difference in the mean age of fallout brought down in different seasons.  相似文献   

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