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1.
Peak activities of radiocaesium (137Cs) in lake sediments have frequently been used to infer the ages of sediments deposited in the 1960s (137Cs derived from nuclear bomb testing) or in 1986 (Chernobyl derived 137Cs). Records of the vertical distribution of 137Cs in sediments can thus be used to provide accurate dates for a critical period in which palaeoecological reconstructions often overlap contemporary monitoring data. However, knowledge regarding how the distribution of 137Cs in sediments is affected by post‐depositional processes is limited to interpretations based on the 137Cs distribution in sediments sampled at a single given date. This study assesses the extent to which the 137Cs record in annually laminated (varved) lake sediments is affected by post‐depositional diffusion, using 11 archived sediment cores sampled between 1986 and 2007. The sediment record reveals how Chernobyl 137Cs incorporated into the 1986 varve diffused downwards in the core at a decreasing rate over time, whereas the surface sediments continued to receive inputs of 137Cs mobilized from the catchment soils or lake margin. In spite of these processes, all cores post‐dating the Chernobyl accident had a clear and well‐resolved peak in the 1986 varve, justifying the use of this feature as a fixed chronostratigraphic feature. Because of the very high levels of Chernobyl fallout at this site, downwards migration of Chernobyl 137Cs has, however, completely masked the nuclear weapons 137Cs fallout peak that had been clearly preserved in the 1964 varve of a pre‐Chernobyl core sampled just three weeks before the Chernobyl accident. In consequence, the weapons fallout marker is likely to be of little use for determining 137Cs dates in areas strongly affected by high levels of Chernobyl fallout.  相似文献   

2.
《Applied Geochemistry》1993,8(5):437-445
The input of137Cs into the troposphere from the Chernobyl nuclear accident made intriguing the use of fallout137Cs as a tool for estimating the rate of soil erosion over Europe. The present paper reports on the adoption of137Cs/134Cs activity ratio to differentiate the vertical distribution of137Cs prioir to and following the Chernobyl accident. The137Cs/134Cs activity ration in the radioactive clouds is required to calculate pre and post- 1986137Cs amounts, considering that the whole134Cs was actually derived from Chernobyl. By using this procedure, the erosion rates could be evaluated for the badland area, the Paglia River basin (central Italy), before and after the Chernobyl accident. Nine sites from two areas of this basin were sampled and analyzed. Erosion rates, ranging from 1.5 to 8.4 mm/a were measured, the values depending both on the basin lithology and site slope. These first results are consistent with those yielded by quantitative geomorphologic methods.  相似文献   

3.
Adsorption of trace amounts of radiocaesium on NH4-, K-, and Na-saturated Fithian illite and subsequent desorption by 1 M NH4 showed that a substantial amount of radiocaesium (44%, 46%, and 91% for NH4-, K-, and Na-illite, respectively) cannot be desorbed after only 5 min of adsorption. Our results suggest that this instantaneous fixation is caused by the collapse of the frayed edges of the clay mineral and the relatively high concentration of radiocaesium building up in solution in the batch desorption experiments. Consequently, commonly applied high-NH4 extractions underestimate truly exchangeable amounts of radiocaesium in soils and sediments containing illitic clay minerals. The rate of desorption of trace amounts of radiocaesium from the solids using high NH4 or Cs concentrations has a half-life of about 2 yr, reflecting radiocaesium desorption from (partially) collapsed interlayers. Extraction of radiocaesium from illite after 5 min of contact time with a Cs-selective adsorbent or a 1 × 10-6 M CsCl solution shows that 100% of the bound radiocaesium is readily available. The desorption rate in the presence of a Cs-selective adsorbent has a half-life of about 0.2 yr. Desorption of radiocaesium from illite using different ammonium concentrations shows that radiocaesium partitioning follows reversible ion-exchange theory if the NH4 concentration is below 1 × 10-4 M, and sufficient time (weeks) is allowed for the reaction to proceed. Thus, radiocaesium sorption reversibility in the natural environment is much higher than generally assumed, and equilibrium solid/liquid partitioning may be assumed for the long-term modelling of radiocaesium mobility in the natural environment. In the particular case of anoxic freshwater sediments with very high NH4 concentrations in the pore waters (up to several mmol.L-1), collapse of the frayed edges of illite may occur, influencing radiocaesium partitioning. If collapse occurs before radiocaesium adsorbs to illite, high caesium sorption reversibility as measured by high-NH4 extraction can be expected because further collapse of the frayed edges during the extraction procedure will be limited. This effect has indeed been observed earlier in the extraction of radiocaesium from anoxic freshwater sediments with high-NH4 solutions and was as yet unexplained.  相似文献   

4.
Cesium-137 derived from the explosion of the Chernobyl reactor in 1986 was preserved in anoxic sediments from a coastal environment in southern Rhode Island. Although the radioactive plume was detected in surface air samples at several locations in the United States, this is the first known record of a Chernobyl 137Cs peak in sediments from North America. The inventory of Chernobyl 137Cs that was preserved in the Pettaquamscutt River is small compared to European counterparts and should only be detectable for the next 15-20 yr. However, the presence of two 137Cs peaks (1963 and 1987) identifies a well-dated segment of the sediment column that could be exploited in understanding the decomposition and preservation of terrestrial and aquatic organic matter. Different methods for calculating the 210Pb chronology were also evaluated in this study and checked against independent varve counting. The end result is a detailed chronology of a site well suited for reconstruction of historical records of environmental change.  相似文献   

5.
Various anthropogenic radionuclides and210Pb were analyzed in a 4.3-m-long core, sampled near the Rhône River mouth in March 1991, to evaluate the extent of industrial releases that accumulate in this area. The whole core was significantly marked by radionuclide inputs from the nuclear facilities located along the river (137Cs,134Cs,60Co). Irregular profiles in natural and artificial radionuclides should be related to variations in their respective inputs from the Rhône River to the Mediterranean Sea. Minimum concentrations were found during high flow periods. Using both the137Cs/134Cs profile in the core and the range of this ratio in Rhône waters, mean apparent accumulation rates were estimated to range between 37 cm yr?1 and 48 cm yr?1. This core would then represent a sedimentary record over a 7–10 year period. However, the presence of a signal from the Chernobyl accident, which occurred on April 26, 1986, was not clearly observed in the core. Inventories of both artificial and natural radionuclides were greater than expected from atmospheric inputs. The increased sedimentation occurring in close vicinity to the mouth of the Rhône River is thus responsible for trapping of elements transported by the river to the Mediterranean Sea. In this area, inventories of artificial radionuclides are well in excess of aerial deposition from Chernobyl and atmospheric weapons tests and are linked primarily to industrial releases.  相似文献   

6.
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   

7.
Sedimentation rate of suspensions (0.3–18.2 mm/yr) was determined on the basis of layer-by-layer distribution of 137Cs (global and Chernobyl) in the cores of bottom sediments (BS) from 16 lakes located in the high and moderate latitudes of the Northern Hemisphere. Profiles of 137Cs concentration in the BS cores were analyzed. Sedimentation rates in the limnic zones of deep-water lakes were calculated using 137Cs accumulated in the finely-dispersed component of mineral suspension.  相似文献   

8.
Four overbank sediment profiles in the Inari area of northern Finnish Lapland were studied in detail by the collection of samples at one-centimetre intervals. The sample sites are situated along a line from northeast to southwest away from the industrial centre at Nikel in the Kola Peninsula. Total, aqua regia and ammonium acetate leachable concentrations were determined for more than 30 elements to study their vertical distribution, and to evaluate the results of the three analytical methods in environmental studies. Radioisotopes of 137Cs and 134Cs were measured on 34 samples to assess radioactive fallout. Radiometrie 14C-dating was determined in one profile to estimate the rate of sedimentation. Grain-size analysis was carried out for calculating the field weight to produce a minimum of 500 g of minus 125 μm material, required for analysis and storage, and to estimate the clay content, which affects leachable element concentrations, when partial or near-total analytical methods are used.It was found that the concentration of studied elements varies with depth. Airborne Ni and S contamination from the smelting plants in the Kola Peninsula was weakly detectable by ammonium acetate leachable contents.137Cs and 134 Cs isotope concentrations, originating from the nuclear weapon tests on the island of Novaya Zemlya and/or from the Chernobyl nuclear power plant accident, were clearly detectable in the topmost layer of overbank sediments. 14C dating has given a time-lag of 5000 years for the deposition of an overbank sediment sequence of 120 cm thickness. Thus, a very slow deposition rate of overbank sediments in northern Finnish Lapland is indicated.It is concluded that grain-size analysis and radiometric dating are necessary for a full interpretation of the geochemistry of overbank sediment sequences, and the selection of leaching methods should be done according to the character of the assumed contamination.  相似文献   

9.
The moment magnitude (M w) 9.0 Tohoku-Oki Earthquake occurred on March 11, 2011, generating an unusually large tsunami. The seismic shocks and tsunami inundation severely damaged the Fukushima Daiichi Nuclear Power Plant. Radionuclide emission due to reactor breakdown contaminated wide areas of Fukushima and its surroundings. Heavy rainfall causes runoff across surface soil, and fine soil particles are susceptible to uptake by the flowing water. The high radioactivity of grains suspended in floodwater indicates that radioactive fallout was streamed into rivers in particulate form and transported downstream under high-flow conditions. Here, we investigated the diachronic mode of 134Cs and 137Cs in central Fukushima, through which the contaminated air mass drifted and caused wet deposition of radionuclides. Stratigraphic measurements of radioactivity in sediment cores is the method employed in this study to determine the basin-wide movement of 134Cs and 137Cs, to evaluate the significance of the erosion–transportation–accumulation processes on natural decontamination in terrain characterized by steep slopes and high precipitation. Stratigraphic results illustrate the process of fluvial sediment discharge, and the massive deposition of radiocaesium suggests basin-wide movement of fallout during concentrated rainfall. Grain suspension in torrential currents is an important pathway for transportation of radionuclides from land to sea, and the appearance of hotspots on floodplains and the offshore sea floor is the consequence of erosion and transportation under seasonal heavy precipitation. Radioactive horizons occur in offshore sediment columns and thus radiocaesium discharged from the estuary will persist forever under the sea floor if no artificial disturbance occurs.  相似文献   

10.
The studies presented explore post-depositional changes of zinc, cadmium, lead, manganese and 137Cs distribution in alluvial sediments accumulated in the upper Odra River valley in southern Poland. The rate of these changes was estimated by comparing metal and 137Cs distributions in four vertical alluvial profiles with a history of river pollution and sediment deposition. The untypical 137Cs distribution with peaks in the surface 40–60 cm and lower down, even at a depth of 2.5 m in strata deposited before the beginning of nuclear tests in 1954, indicates rapid post-depositional migration of this isotope from the surface and its retention in lower, less permeable layers. Moreover, the highest concentrations of lead, zinc and cadmium were found at a depth of 4 m in sediments accumulated in the mid-nineteenth century in spite of the growth of industrialization and the pollution of the Odra River with heavy metals until the end of the twentieth century. The post-depositional changes in heavy metals and 137Cs are rapid in comparison with the slow element migration usually observed in uninundated soils. This difference is explained by the frequent and easy infiltration of polluted river water into the gravelly and sandy sediments present in the profiles.  相似文献   

11.
The redistribution of Chernobyl 137Cs within a small drainage basin was studied in the Lokna river basin, Tula region, Central Russia. Sheet erosion on the cultivated part of basin is the main reason for 137Cs horizontal migration. However there is no statistically significant 137Cs redistribution within cultivated field because of relatively low erosion rates. The valley bottom is the main sink of 137Cs, where 73–84% eroded soil is stored. The resulting 137Cs level in the valley bottom is 1.5–2 times that of the initial 137Cs fallout.  相似文献   

12.
Anthropogenic radionuclides (137Cs,134Cs,60Co) have been introduced to the James River estuary as a result of low-level releases from the Surry Reactor site since 1973 and worldwide atmospheric fallout from nuclear weapons tests since the early 1950s The total radionuclide burden in the estuary sediments has been estimated by integrating radionuclide activities in 29 box cores and extrapolating these integrated values over surface areas subdivided on the basis of sediment type, rates of accumulation, and proximity to the reactor release site. Our results indicate that 30% of the60Co, but only 15% of the134Cs released from the reactor site, has been retained in the estuary sediments, and about 40% of the134Cs and60Co sediment inventory is in areas that represent less than 5% of the total estuarine surface area. Depletion of the134Cs in downstream sediments forms a noticeable trend in the James River estuary, and we postulate that seawater cation competition and exchange is primarily responsible.  相似文献   

13.
Reliable dating is an essential element of palaeoseismological studies, yet whilst a suite of geochronological methods can now provide late Quaternary age control it remains very difficult to date modern events (i.e., those occurring within the last 150 years). This is significant because the starting point for many palaeoseismological investigations is a modern surface-rupturing event, whose geological effects need to be disentangled in trench stratigraphies from palaeoseismic ruptures. Two dating methods which, in combination, can provide robust dating control in recently deposited sediments are the 210Pb and 137Cs dating methods. Here, we test the applicability of using 210Pb and 137Cs to date colluvial sediments exposed in three trenches excavated across an earthquake fault—the Eliki fault, Gulf of Corinth, Greece—which ruptured in an earthquake in 1861. The 210Pb and 137Cs profiles observed in these colluvial sequences are relatively erratic due to the mixed nature of the sediments, i.e., their deposition in an environment where the supply of slope sediments is driven by seasonal rainfall, causing non-uniform sediment accretion and sediment reworking. In one trench, however, 210Pb dating, corroborated by 137Cs dating, indicates that a proposed post-1861 surface colluvial unit has been deposited over the period 1950 AD–present (at a rate of ca. 9 mm/year), and overlies a significantly older unit (>120 years old). The dating control provided here by 210Pb and 137Cs dating corroborates the published interpretation of the trench stratigraphy, and refines the 14C-based estimated dates for the upper unit. At two other trenches 210Pb and 137Cs dating only provided minimum ages (based on the presence or absence of 210Pbexcess and 137Cs). Such approximate ages, however, may still useful in corroborating interpretations made using the trench stratigraphy, or, at sites which have long earthquake recurrence intervals, determining which earthquake event was responsible for a particular bed offset.  相似文献   

14.
 This study was undertaken to determine whether recent anthropogenic changes in the Nile basin have affected the modern rate of sediment accumulation in the Nile delta. Excess 210Pb, 137Cs, and 239,240Pu were used to develop a sediment chronology for a core from central Manzala lagoon, the delta sector which has had the highest average rate of sediment accumulation during the Holocene (to about 0.7 cm year–1). Excess 210Pb was detected in the top 32 cm of the core, yielding an accumulation rate of 1.2 cm year–1, higher than the mean rate for the Holocene. A high 137Cs/239,240Pu ratio requires a reactor source (possibly Chernobyl) for these nuclides. Low concentrations of excess 210Pb and weapons-fallout nuclides precluded recognition of changes in sediment accumulation rate in Manzala lagoon during this century and may limit the use of tracer radionuclides for modern sediment chronology in the Nile delta. Received: 18 March 1997 · Accepted: 22 July 1997  相似文献   

15.
《Applied Geochemistry》1998,13(2):155-164
Two issues are addressed in this paper: the solid/liquid distribution behaviour of radiocaesium (137Cs and 134Cs) and radiostrontium (90Sr) in sapropels, and the potential effectiveness of sapropels as amendments to remediate soils contaminated with these radionuclides. It is shown that the solid/liquid partitioning of radiocaesium and radiostrontium in sapropels is governed by the same processes as in soils. Experimental KD values measured in a representative solution vary between 300 and 5000 dm3 kg−1 for radiocaesium and between 15 and 50 dm kg−1 for radiostrontium. These KD values can be interpreted quantitatively on the basis of the main factors which govern the solid/liquid partitioning of these radionuclides.This quantitative approach also allows predictions to be made on the potential effectiveness of sapropel amendments in contaminated soils. These predictions agree very well with experimental results from simple laboratory experiments aimed at investigating the amendment effect. Addition of 1–4 wt.% doses of 2 sapropel samples with different radiocaesium retention characteristics had no significant effect on the radiocaesium distribution coefficient in sandy soils. It is therefore expected that the addition of such sapropels will not result in a decrease of the radiocaesium soil-to-plant transfer, at least not from the point of view of the increase of the radiocaesium retention in the amended soil. Addition of 1–4 wt.% doses of a high CEC sapropel to low CEC sandy soils increased the radiostrontium distribution coefficient up to 3.5 times. It can thus be expected that addition of such high CEC sapropel will increase the radiostrontium retention in the amended soil, and thus decrease the radiostrontium soil-to-plant transfer.  相似文献   

16.
The Candamo Cave contains an important group of paleolithic paintings which have been seriously deteriorated due to mass tourism. In this work, an analysis was carried out of different climatic parameters (CO2, temperature, humidity, 222Rn) during annual cycles with the cave closed to the public and during an experimental period of controlled visits. The effect of visits on the geochemical characteristics of karstic water was also analyzed together with the cave ventilation. The natural variations in the cave air CO2 were above 3000 ppm, the increase produced through visits was only 100–110 ppm and since the humidity is almost permanently at saturation point, the critical parameter which limits the visitor capacity becomes air temperature. The temperature changes during the annual cycle are of the order of 1  °C in the external part and less than 0.5  °C in the internal part of the cave and a maximum increase of 0.13  °C was observed during the period of the visits. The 222Rn and CO2 concentration minimums in the summer period (July–October) show that this is the most propitious time for visits, since the greatest ventilation is produced in the cave at this time and, therefore, the greatest capacity for recovery. The geochemistry of the water, on the other hand, indicated that this is the period of the year in which processes of wall corrosion can be most easily introduced, although this would be of limited magnitude. The visitor capacity calculated was 29 visitors/day. Received: 29 August 1996 · Accepted: 23 June 1997  相似文献   

17.
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   

18.
Vertical profiles of 137Cs and 239,240Pu were measured in soils collected from two sites in southern Sweden and three sites in southern Poland and were modeled using both a solute transport model and a bioturbation model to better understand their downward migration. A time series of measured 137Cs profiles indicates that 137Cs from Chernobyl was found at the soil surface in 1986 but it has migrated progressively downward into the soil 4.5-25.5 cm since. However, because of dispersion during the migration and mixing following Chernobyl deposition and the much higher activities of 137Cs from Chernobyl, stratospheric fallout of 137Cs from the 1960s cannot be identified as a second 137Cs activity maximum lower in the soil column at any of the sites. Conversely, the 240Pu/239Pu ratio indicates that no Chernobyl-derived Pu is present in any of the cores with the exception of one sample in Sweden. This difference may be attributed to the nature of the release from Chernobyl. Cesium volatilized at the reactor temperature during the accident, and was released as a vapor whereas Pu was not volatile and was only released in the form of minute fuel particles that traveled regionally. Both the solute diffusion and the bioturbation models accurately simulate the downward migration of the radionuclides at some sites but poorly describe the distributions at other sites. The distribution coefficients required by the solute transport model are about 100 times lower than reported values from the literature indicating that even though the solute transport model can simulate the profile shapes, transport as a solute is not the primary mechanism governing the downward migration of either Cs or Pu. The bioturbation model uses reported values from the literature of the distribution coefficients and can simulate the downward migration because that model buries the fallout by placing soil from depth on top and mixing it slightly throughout the mixing zone (0.6-2% per year of mixing). However, mixing in that model predicts concentrations in the top parts of the soil profiles which are too high in many cases. Future progress at understanding the downward migration of radionuclides and other tracers will require a more comprehensive approach, combining solute transport with bioturbation and including other important soil processes.  相似文献   

19.
Controlled laboratory experiments have been used to study the diagenetic chemistry of 239,240Pu 137Cs, and 55Fe. Experiments using Buzzards Bay sediments in small tanks show that sulfate reduction is accompanied by the production of large pore water concentration gradients of alkalinity, phosphate, ammonia and dissolved organic carbon and the formation of subsurface maxima in Fe and Mn. These pore water profiles demonstrate that bacterially-mediated processes of organic matter degradation and redox reactions can be simulated in the laboratory.A vertical profile of 55Fe in pore waters is reported for the first time: it follows the profile of stable Fe and as such has a large (200 dpm/100 kg) subsurface maximum between 2–4 cm depth. Comparison of 55Fe/Fe ratios in sediments and pore waters shows that there is preferential solubilization of 55Fe over stable Fe.The pore water activities of 239,240Pu show no gradients within the large uncertainties of the counting statistics, but are two to four times higher than Buzzards Bay seawater (0.05 dpm/100 kg).The activity of 137Cs in the pore water profile is constant (40 dpm/100 kg) within the large counting uncertainties and is twice that of Buzzards Bay seawater. Cs-137 does not appear to be involved in diagenetic chemistry but may increase in pore waters as a result of ion exchange reactions.Flux estimates based on the pore water data show that remobilization and transport of 239,240 Pu in coastal sediments are not significant processes while the transport of l37Cs may be.  相似文献   

20.
Recent identification of elevated excess 210Pb (≤302.6 mBq L−1) and 137Cs (≤111.3 mBq L−1) activity in drinking water wells up to 20 m depth indicates some transport of airborne radionuclide fallout beyond soils in the Shaker Village catchment, Maine. Estimated airborne mass loading 210Pbex fluxes of about 0.9 mBq m−3, canvass this headwater catchment and may be sufficient to pose risks to unprotected shallow wells. Inventories of 210Pbex and 137Cs in pond sediments indicate maximum median activities of 943 mBq g−1 and 40.0 mBq g−1, respectively. Calculated 210Pbex fluxes in the catchment soils range from 0.62–0.78 Bq cm−2 year−1 and yield a mean residence time of near 140 years. Measured 137Cs activity up to 51.1 mBq g−1 occurs in sediments at least to 5 m depth. Assumed particle transport in groundwater with apparent 85Kr ages less than 5 years BP (2005) may explain the correlation between these particle-reactive radionuclides and elevated activity in some drinking water wells.  相似文献   

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