The occurrence and bioavailability of radioactive 137Cs in small forest lakes in Southern Finland

Following the Chernobyl accident in late April 1986, central Finland was subjected to considerable radioactive fallout. The radioactive isotope of caesium, (137)Cs, was potentially the most harmful isotope in the fallout because of its long half-life (30 years). (137)Cs activities remained unexpectedly low within the biota (algae, zooplankton, aquatic moss, fish) of some humic forest lakes in southern Finland compared to the clear water lakes within the same district. This observation suggested that humic substances, by binding (137)Cs chemically, may reduce its bioavailability in lake water. Our laboratory experiments (throughflow systems; gel chromatography) demonstrated that binding of (137)Cs by humic substances was negligible in untreated lake waters; only when most of the alkali metals had been removed with an ion exchange resin was any binding of (137)Cs by low molecular humic fractions apparent. Instead, the concentrations of cations (especially potassium) were of overwhelming importance for the bioavailability of (137)Cs within the lacustrine ecosystems. The concentrations of (137)Cs within food chains are expected to stay at a high level for many years especially in lakes with long water renewal times.     

Ecological half-life of caesium in roe deer (Capreolus capreolus)

Biological half-lives for various radionuclides have been determined for many animals kept in the laboratory or under controlled conditions. Only occasionally has been it possible to determine the ecological half-lives of radionuclides in wild animals, where the contamination has occurred in their natural habitats. Following the fallout from the Chernobyl accident and its subsequent ingestion by wildlife, no one knew how long it would take the wild animals to eliminate the radionuclides, and in particular radiocaesium, from their bodies. In this study of roe deer (Capreolus capreolus), bucks (males)were shot at weekly/fortnightly intervals from mid-May till the end of July, as part of the annual cull on an area, which included some young forestry (Stone Chest-National Grid Reference NY48090), planted in 1971/72. The ration of 137Cs:134Cs, typical of the Chernobyl fallout, was seldom observed in these animals due to the highly variable concentrations of 137Cs originating from bomb fallout. Therefore, 134Cs was used instead because its presence was almost entirely due to the Chernobyl fallout. After using log10 transformation of the 134Cs concentrations, a significant (p < 0.01) regression was obtained which accounted for 85% of the variation. From the regression, the ecological half-life for 134Cs was found to be 28.3 days.     

Radiocaesium activity concentrations in potatoes in Croatia after the Chernobyl accident and dose assessment

Systematic investigations of (137)Cs and (134)Cs activity concentrations in potatoes (Solanum tuberosum) for the post-Chernobyl period (1986-2005) in the Republic of Croatia are summarized. The correlation between (137)Cs activity concentrations in fallout and potatoes, has been found to be very good, the correlation coefficient being r = 0.88 with P(t) < 0.001 for 18 degrees of freedom. As the radiocaesium levels in potatoes decreased exponentially, the mean residence time of (137)Cs in potatoes was estimated by fitting the measured activity concentrations to the exponential curve. The mean residence time was found to be 6.8 +/- 1.1 years, the standard deviation being estimated by the Monte Carlo simulations. The initial observed (134)Cs:(137)Cs activity ratio in potatoes has been found to be quite variable, but slightly lesser than the theoretically predicted value of 0.5, calculated by applying the known inventory of these radionuclides in the Chernobyl reactor to the equation for the differential radioactive decay. This can be explained by presence of the pre-Chernobyl (137)Cs in soil that originated from nuclear fallout. The annual effective doses received by (134)Cs and (137)Cs intake due to consumption of potatoes estimated for an adult member of the Croatian population were found to be very small, as the per caput Dose for the entire 1986-2005 period was calculated to be about 2.9 microSv, (134)Cs accounting approximately for 1/3 of the entire dose. Therefore, after the Chernobyl accident consumption of potatoes was not the critical pathway for human intake of radiocaesium from the environment in Croatia.     

Accumulation history of radionuclides in the lichen Stereocaulon vesuvianum from Mt. Vesuvius (south Italy)

The fruticose lichen Stereocaulon vesuvianum, growing on the slopes of Mt. Vesuvius (south Italy), was used as a biomonitor of 134Cs, 137Cs, 103Ru and 106Ru derived from the April 26 1986 Chernobyl nuclear reactor accident. Samples were taken at five different quotes (370, 490, 580, 780 and 960 m a.s.l.) and four successive dates (October 1986, December 1986, October 1987 and May 1999). At the first sampling, the concentrations (as Bq kg(-1) dry weight) ranged between 460 and 1020 for 134Cs, 1330 and 2500 for 137Cs, 90 and 200 for 103Ru and 360 and 710 for 106Ru, values generally lower in respect to those measured in soil and higher plants. Of the total 137Cs measured only 14% was due to 1950s and 1960s nuclear weapons tests fallout. Highest average activities of all nuclides were observed at the quote of 960 m and significant correlation (0.7相似文献   

Long term investigation of 137Cs in chicken meat and eggs from northwest Croatia

Abstract

This paper presents the results of long-term investigations of ¹³⁷Cs activity concentrations in chicken meat and eggs from northwest Croatia for the period 1987–2018. The research has been done as a part of monitoring program of radioactive contamination in Croatia. The highest activity concentrations in both of these foodstuffs were measured in 1987 and have been decreasing exponentially ever since. The Fukushima-Daiichi accident in 2011 did not cause any increase of ¹³⁷Cs activity concentrations. The ecological half-life for ¹³⁷Cs was estimated to be 8.0 and 8.4?years for chicken meat and eggs respectively. The correlation between ¹³⁷Cs in fallout and chicken meat as well as between ¹³⁷Cs in fallout and eggs is very good, the respective correlation coefficients being 0.79 and 0.72, indicating that fallout was the main source of ¹³⁷Cs contamination in both foodstuffs. The estimated effective doses received by adult members of the Croatian population due to the intake of radiocaesium by chicken meat and egg consumption for the overall observed period are very small, 2.0 and 0.6 µSv respectively. Therefore, chicken meat and chicken egg consumption was not a critical pathway for the transfer of radiocaesium to humans.     

Rates of removal of sediment associated radiocaesium from the plynlimon experimental catchments, Powys, UK

Inventories of weapons-test and Chernobyl derived (137)Cs within the upper Wye and upper Severn catchments have been estimated using a variety of techniques. Transport rates of radiocaesium from the catchments have been determined from measurements of radionuclide activities on suspended and bedload sediments. Radiocaesium transport coefficients calculated from the results of 0.46-5.42 x 10(-3) y(-1) for freshly deposited Chernobyl (137)Cs contrast with that for older weapons-test fallout (137)Cs deposits (0.035-0.36 x 10(-3) y(-1)). These results show that freshly deposited Chernobyl (137)Cs is presently being lost at a significantly higher rate than weapons-test derived (137)Cs. For (137)Cs from both sources, residence times in the undisturbed upper Wye catchment are significantly higher than in the afforested upper Severn catchments.     

Transfer of radioactive caesium from soil to vegetation and comparison with potassium in upland grasslands

The distribution and transfer of caesium and potassium between soils and vegetation has been investigated by field sampling and experimental studies on soils and vegetation typical of upland grassland in north west England. Total (137)Cs content to a depth of 0.05 m below root matt ranged from 13 000 to 18 000 Bq m(-2). This caesium content derives from three sources: the Windscale accident of 1957, weapons-testing fallout which peaked in the early 1960s, and the Chernobyl accident in May 1986. From 2200 to 6200 Bq m(-2) is attributed to the first two sources, and the remainder to Chernobyl. In December 1986, 23-78% of pre-Chernobyl (137)Cs was associated with soil underlying root matt and 0.5-5.5% was associated with vegetation. Plant/soil concentration ratios for pre-Chernobyl (137)Cs were in the range 0.5-6.5, the lowest values being associated with patches of Festuca/Agrostis turf. At the same time, 4-19% of (137)Cs deposited from Chernobyl was associated with vegetation, although higher values appeared in conjunction with the moss, Polytrichum commune. Corresponding total potassium contents were in the range 9.6-22 mg m(-2) to 0.05 m soil depth. Lower values were found at the wetter sites where, on average, 5.7% of the total potassium was present in vegetation. At drier sites the potassium content was higher and, on average, 8.9% was present in vegetation. Plant/soil concentration ratios ranged from 2.2 to 9.2. During accelerated growth of vegetation, on monoliths in glasshouse conditions over the winter of 1986/87, (137)Cs was transferred from soil and root matt to new growth, such that concentrations in fresh growth were similar to or higher than those observed in the field during December 1986. Removal of caesium by successive cuts resulted in up to 25% of the original estimated total being removed over a 240 day period. Increased concentrations coincided with the emergence of Carex sp. and Trichophorum caespitosum, as well as the development of Agrostis sp. and Festuca ovina. Observed Cs/K discrimination ratios, particularly for (137)Cs deposited from Chernobyl, were higher than previously reported in the literature. The experimental results were confirmed by field observations during spring 1987 and it is concluded that caesium deposited as a result of the Chernobyl accident will continue to be recycled in organic and low potassium soils.     

Global fallout Pu recorded in lacustrine sediments in Lake Hongfeng, SW China

Studies on the distribution and isotope compositions of fallout Pu are important for source characterization of possible future non-fallout Pu contamination in aquatic environments, and useful for dating of recent sediments to understand the pollution history of environmental contaminants. We present the historical record of atmospheric Pu fallout reconstructed from a sediment core from Lake Hongfeng, China. The Pu activity profile was in agreement with the 137Cs profile. Inventories were 50.7 Bq m(-2) for 239+240Pu and 1586 Bq m(-2) for 137Cs. The average 240Pu/239Pu atom ratio was 0.185+/-0.009, indicating that Pu originated from global stratospheric fallout rather than from direct tropospheric or close-in fallout from the Chinese nuclear testing conducted in the 1970s. Our data suggested that Lake Hongfeng would be an ideal setting for monitoring atmospheric fallout and environmental changes in this region.     

Constraints on the use of 137Cs as a time-marker to support CRS and SIT chronologies

CRS and SIT are two (210)Pb-based models widely used in the radiometric dating of recent sediments. (210)Pb chronologies should be validated using at least one independent tracer, such as (137)Cs. This paper demonstrates that simple methods based on the identification of (137)Cs fallout peaks cannot provide a definitive support for CRS and SIT chronologies. Two main arguments will support this assertion: Firstly, the (137)Cs time-marks cannot support a CRS or SIT chronology if the derived sedimentation rates cannot explain the whole (137)Cs activity profile without postulating mixing. Secondly, the support by the (137)Cs time-marks for a given CRS or SIT chronology cannot be considered as definitive if other dating models can equally explain the whole set of data, thereby producing a different chronology. Several case studies selected from the literature are used to support the present discussion.     

Sources and pathways of artificial radionuclides to soils at a High Arctic site

Activity concentrations, inventories and activity ratios of ¹³⁷Cs, ²³⁸Pu, ^239?+?240Pu and ²⁴¹Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m² for ¹³⁷Cs, ²³⁸Pu, ^239?+?240Pu and ²⁴¹Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The ²³⁸Pu/^239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The ²³⁸Pu/^239?+?240Pu and ^239?+?240Pu/¹³⁷Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.     

Excess plutonium in soil near the Nevada Test Site,USA

Two soil profiles were collected from undisturbed areas near the Nevada Test Site (NTS). The activity of 137Cs in the surface layer of the downwind Queen City Summit profile is three times higher than at the upwind site at Searchlight, NV (41.1+/-0.6 mBq/g vs. 13.0+/-0.4 mBq/g), and the 239,240Pu activity is 100 times greater (51+/-2 mBq/g vs. 0.52+/-0.03 mBq/g). An examination of the literature suggests that the 137Cs/239,240Pu and the 239,240Pu/238Pu activity ratios in soils and sediments from the northern hemisphere, due to fallout from atmospheric atomic weapons testing, have generalized values of 36+/-4 and 30+/-4, respectively (as of 1 July 1995). Deviations from these values may indicate possible contamination by sources other than fallout. Data from the surface soil of the downwind Queen City Summit profile yield a 137Cs/239,240Pu ratio of 0.81+/-0.02 and a 239,240Pu/238Pu ratio of 78+/-6. Clearly, an increase in 239,240Pu relative to 137Cs or 238Pu can account for these observations. There is compelling evidence that this "excess" 239,240Pu came from activities at the NTS during the aboveground testing of nuclear devices, more than likely from safety tests, some 40 years ago, and/or during the interim by the wind-driven resuspension of contaminated surface soil on the NTS and its transport off-site. Moreover, the two concentration profiles show that high percentages of both of these elements are retained for decades in the upper few centimeters of soil in Nevada's desert environment.     

Lower variability of radionuclide activities in upland dairy products compared to soils and vegetation: implication for environmental survey

Contamination of the environment by radionuclides is usually estimated using soil and grass sampling. However, radionuclides are often not homogeneously distributed in soils. In the alpine Mercantour region (Western Alps, France) a large heterogeneity in Chernobyl 137Cs deposition has been previously observed. Here we report additional 137Cs results together with new 90Sr and Pu data for soil, grass, milk, and cheese samples. The results show that radioisotopes from nuclear weapons tests fallout are more homogeneously distributed than Chernobyl 137Cs. Further, we observe that the 137Cs and 90Sr contents are less variable in milk samples than in grass or soil samples. This can be attributed to the homogenization effect of cow vagrancy during grazing. Hence milk seems to be a more robust sample than soil or grass to evaluate the extent of contamination on a regional scale. We explore this idea by comparing own unpublished 90Sr results and 90Sr results from the literature to establish the relationship between altitude of grazing and contamination of soil and milk for Western Europe. There is a significant positive correlation between soil contamination and altitude and an even closer correlation between milk 90Sr activity (A) and altitude (h): A = A0 + e(k x h) where A0 is the expected activity of milk sampled at sea level (A0 = 0.064 +/- 0.014 Bq g(-1) Ca) and h is the altitude of grazing, k being a constant (k = 0.95 x 10(-3) +/- 0.11 x 10(-3) m(-1) Bq g(-1) Ca). The fact that there is less scattering in the relationship for the 90Sr(milk)-altitude than for 90Sr(soil)-altitude suggests, again, that milk is a well-suited sample for environmental survey. The relationship between the altitude of grazing and the 90Sr content of milk and cheese can also be used to assess the authenticity of dairy products.     

Laboratory analyses of 137Cs uptake by sunflower, reed and poplar

The 137Cs uptake by three plant species (Phragmites australis L., Heliantus annus L., Populus simonii L.) was analyzed in a hydroponic medium (14 MBql(-1); 0.5 mM CsCl) during cultivation. The radioactivity disappearance from the medium was measured after 2, 4, 8, 16 and 32 days of cultivation. Radioactivity distribution within the plant was determined by autoradiography. We did not find differences between uptake of radioactive and stable caesium isotopes. Relations between the uptake of 137Cs and concentration of potassium and ammonium ions in medium were also tested. The highest uptake of radiocaesium by sunflower was obtained for medium with 1 mM K2SO4 (14.2%) and in case of ammonium ions for concentration ratio 6 mM NH4Cl : 3 mM NH4NO3 (13.2%). The obtained results make it possible to compare the capability and rate of 137Cs phytoremediation of different plant species.     

Concentration of global fallout 99Tc in rice paddy soils collected in Japan

Analysis of global fallout 99Tc in environmental samples should provide useful information for predicting the nuclide behaviour under natural conditions which is important from the viewpoint of radioecology. Concentrations of 99Tc in rice paddy soils collected in Japan have been studied. After chemical separation, 99Tc in the final solution was measured by ICP-MS. The activity ratio of 99Tc/137Cs was used to understand the 99Tc behaviour in the environment because the fission yields of 99Tc and 137Cs from 235U or 239Pu are almost the same. The theoretical activity ratio from fission which is calculated now is about 3.0 x 10(-4). Our results showed that the range of activity ratios of 99Tc/137Cs in the soil samples was (2.0-5.2) x 10(-3); these ratios were one order of magnitude higher than the theoretical one. 99Tc has been accumulating in rice paddy soil like 137Cs has, although their mechanisms might differ. One of the reasons for the high ratio in the surface soil might be the ratios in the atmospheric samples, which have increased from the order of 10(-3) to 10(-2) (García-León et al., 1993).     

Soil-to-plant and plant-to-cow's milk transfer of radiocaesium in alpine pastures: significance of seasonal variability

Because our present knowledge on the environmental behaviour of fallout radiocaesium in semi-natural environments is rather limited, the transfer of this radionuclide and of natural 40K, from soil-to-plant as well as from plant-to-cow's milk was investigated for a typical alpine pasture (site P). For comparison, a nearby alpine pasture (site K) not used for cattle grazing was also studied. Small seasonal effects were found for 137Cs in the plants, but they were different for the two pastures. Due to the presence of a large variety of different plant species on the pastures and soil adhesion on the vegetation from trampling cattle, the scattering of the data was very large, and the seasonal effects were observable only because of the large number of samples (N approximately 100) collected. The aggregated soil-to-plant transfer factor of 137Cs was for site P, on average, 0.002 +/- 0.001 m2 kg(-1). The plant-to-milk transfer coefficient was, on average, 0.02 day l(-1). The 137Cs concentration in the milk of the cows varied within the grazing period only between 1.4 and 2.9 Bq l(-1), with a significant maximum in the beginning of August. As a result of soil adhesion due to cattle trampling, significantly higher ash- and 137Cs contents of the plants were observed at site P as compared to site K. Possible consequences of the above observations with respect to a representative sampling design of vegetation and milk are discussed.     

PCBs and HCHs in a salt-marsh sediment record from South-Central Chile: use of tsunami signatures and 137Cs fallout as temporal markers

This paper documents the occurrence of polychlorinated biphenyl (PCB) and hexachlorocyclohexane (HCH) deposition inferred from a sedimentary record exposed in a salt-marsh trench in South-Central Chile. Sediments were carefully collected every 1 cm from the trench wall. The samples were analyzed for PCBs, HCHs, 137Cs, organic carbon and grain size. The 137Cs fallout and the sedimentary signature left by the 1960 Chilean tsunami were used as temporal markers to estimate the stratigraphic chronology and the sedimentation rates. PCBs were quantified by gas chromatography with electron capture detection (GC-ECD), and positive samples were confirmed by gas chromatography and mass spectrometry detection (GC-MS). Based on these results, PCBs and HCHs deposition over the last 40 years was estimated. No PCBs were detected below the tsunami signature. Total concentrations ranged from undetectable (ND) to 32 ng/g d.w. for PCBs and from undetectable (ND) to 1.29 ng/g d.w. for HCHs. The highest PCB concentrations were found in the upper 7 cm of the core. Even though PCBs were banned in 1982 as electrical fluids in Chile, total estimated PCB fluxes have increased approximately 20 times during the last 40 years: from undetectable values to 102.6 ng/cm2/year, reflecting that PCBs are still in use and being released into the environment.     

Cesium-137 and mercury contamination in lake sediments.

The contribution of fluvial discharge and global fallout of 137Cs and mercury to sedimentation fluxes in Lake Shinji and Lake Nakaumi, Japan, was studied. The fluvial flux through soil erosion accounted for 11 to 27% of accumulated 137Cs in the sediments in the 1950's and 1960's, which were the periods of the most extensive atmospheric input, and for 90 to 100% in the 1990's. The vertical profiles of mercury concentrations in the lake sediments studied showed a maximum between 1959 and 1963, which was originated mostly from the extensive use of mercury-agrochemicals in paddyfields of the watershed in the past. These findings are representative examples of long-term contamination of lake sediments caused by the contaminated ground soil erosion.     

Distribution coefficients (Kd) and desorption rates of Cs and Am in Black Sea sediments

The distribution coefficients (K_d) and desorption rates of ¹³⁷Cs and ²⁴¹Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The K_d values were found to be 500 for ¹³⁷Cs and 3800 for ²⁴¹Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for ¹³⁷Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of ¹³⁷Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of ²⁴¹Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the ²⁴¹Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than ¹³⁷Cs under Black Sea conditions.     

Dynamic equilibrium of radiocesium with stable cesium within the soil-mushroom system in Turkish pine forest

Mushrooms and soils collected from pine forests in Izmir, Turkey were measured for radiocesium and stable Cs in 2002. The ranges of (137)Cs and stable Cs concentrations in mushrooms were 9.84+/-1.67 to 401+/-3.85Bqkg(-1) dry weight and 0.040+/-0.004 to 11.3+/-1.09mgkg(-1) dry weight, respectively. The concentrations of (137)Cs and stable Cs in soils were 0.29+/-0.18 to 161+/-1.12Bqkg(-1) dry weight and 0.14+/-0.004 to 1.44+/-0.045mgkg(-1) dry weight, respectively. Even though different species were included, the concentration ratios of (137)Cs to stable Cs were fairly constant for samples collected at the same forest site, and were in the same order of magnitude as the (137)Cs to stable Cs ratios for the organic soil layers. The soil-to-mushroom transfer factors of (137)Cs and stable Cs were in the range of 0.19-3.15 and 0.17-12.3, respectively. The transfer factors of (137)Cs were significantly correlated to those of stable Cs.     

The influence of season and leaf age on concentrations of radiocaesium (137Cs), stable caesium (133Cs) and potassium in Agrostis capillaris

The transfer of radioactive caesium from soils to plants has been well researched. In contrast there is limited knowledge on natural stable 133Cs and its potential role as a predictor for radiocaesium behaviour. In a pot experiment with Agrostis capillaris close correlations were found between plant 137Cs and plant 133Cs concentrations (R2 90-96%). Season and leaf age had significant effects with concentrations increasing 10-30-fold between June and December. Simultaneously the plant concentrations of K, the nutrient analogue of Cs, decreased to around one third. In the soil the exchangeable fractions of K and 137Cs declined. No clear relationships were found between 137+133Cs in the plant and exchangeable K in the soil. However, at the end of the experiment the K content of the above-ground biomass was higher than the exchangeable pool in the soil, suggesting that depletion of soil K could be a key factor in the observed increase of plant 137+133Cs over time.