Association of plutonium with sediments from the Ob and Yenisey Rivers and Estuaries

The present study applied sequential extraction techniques to investigate the binding and mobility of plutonium (Pu) in sediments from the rivers and estuaries of the Ob and Yenisey. As a study site, the Ob and Yenisey are particularly interesting as both rivers have weapons-grade Pu sources in their catchment areas, including the Russian Pu production and reprocessing plants at Mayak, Tomsk-7 and Krashnoyarsk, and the Semipalantinsk nuclear weapons testing site in Kazakhstan. Plutonium activity and ²⁴⁰Pu/²³⁹Pu ratios were determined using accelerator mass spectrometry (AMS). Sequential extractions showed that between 47 and 80% of the Pu in Yenisey River sediments and 35–53% of the Pu in soils around the Techa River are mobilized with weak oxidising agents, which can indicate that Pu is bound to organic material. In contrast, Pu in Ob and Yenisey Estuarine sediments was more strongly bound, with 60–100% being found in the HNO₃-extractable fraction. This change in speciation could reflect either that Pu bound to organic material in the Techa and Yenisey River sediments becomes more fixed to the sediments with time, or that organic-bound Pu is mobilized and released to the water when the sediments encounter the more saline water of the Ob and Yenisey estuaries. In general, ²⁴⁰Pu/²³⁹Pu ratios were relatively consistent between different extraction fractions, although, in whole sediments, an increase in ratio was observed with distance from the source. This reflects the increased influence of weapon fallout from catchment runoff within the river systems, as compared to the weapons-grade sources close to the production and reprocessing plants. Knowledge of Pu speciation in the Ob and Yenisey Rivers, and the processes controlling its behaviour in estuarine systems, can improve predictions of its transfer and subsequent environmental impact to Arctic Seas.     

Cs uptake by four plant species and Cs-K relations in the soil-plant system as affected by Ca(OH)2 application to an acid soil

Three rates of Ca(OH)₂ were applied to an acid soil and the ¹³⁴Cs uptake by radish, cucumber, soybean and sunflower plants was studied. The ¹³⁴Cs concentration in all plant species was reduced from 1.6-fold in the sunflower seeds to 6-fold in the soybean vegetative parts at the higher Ca(OH)₂ rate. Potassium (K) concentration in plants was also reduced, but less effectively. The significantly decreased ¹³⁴Cs-K soil to plant distribution factors (D.F.) clearly suggest a stronger effect of soil liming on ¹³⁴Cs than on K plant uptake. This observation was discussed in terms of ionic interactions in the soil matrix and within the plants. The results also indicated that the increased Ca²⁺ concentration in the exchange phase and in the soil solution along with the improved root activity, due to the soil liming, enhanced the immobilization of ¹³⁴Cs in the soil matrix and consequently lowered the ¹³⁴Cs availability for plant uptake.     

Plutonium concentrations in waters from the southern Baltic Sea and their distribution in cod (Gadus morhua) skin and gills

The concentrations of (238)Pu and (239+240)Pu in water samples and suspended particulate fractions, as well as in colloidal fraction from the southern Baltic Sea are presented. The (239+240)Pu concentration in surface seawater samples fall within range from 5.2 mBq.m(-3) for Gdańsk Bay to 150 mBq.m(-3) for Pomeranian Bay, most of which (from 52 to 96%) constituted filterable forms (相似文献   

Upward movement of plutonium to surface sediments during an 11-year field study

An 11-year lysimeter study was established to monitor the movement of Pu through vadose zone sediments. Sediment Pu concentrations as a function of depth indicated that some Pu moved upward from the buried source material. Subsequent numerical modeling suggested that the upward movement was largely the result of invading grasses taking up the Pu and translocating it upward. The objective of this study was to determine if the Pu of surface sediments originated from atmosphere fallout or from the buried lysimeter source material (weapons-grade Pu), providing additional evidence that plants were involved in the upward migration of Pu. The ²⁴⁰Pu/²³⁹Pu and ²⁴²Pu/²³⁹Pu atomic fraction ratios of the lysimeter surface sediments, as determined by Thermal Ionization Mass Spectroscopy (TIMS), were 0.063 and 0.00045, respectively; consistent with the signatures of the weapons-grade Pu. Our numerical simulations indicate that because plants create a large water flux, small concentrations over multiple years may result in a measurable accumulation of Pu on the ground surface. These results may have implications on the conceptual model for calculating risk associated with long-term stewardship and monitored natural attenuation management of Pu contaminated subsurface and surface sediments.     

Plutonium(VI) accumulation and reduction by lichen biomass: correlation with U(VI)

The uptake of plutonium(VI) and uranium(VI) by lichen biomass was studied in the foliose lichen Parmotrema tinctorum to elucidate the migration behavior of Pu and U in the terrestrial environment. Pu and U uptake by P. tinctorum averaged 0.040+/-0.010 and 0.055+/-0.015 g gdry (-1), respectively, after 96 h incubation with 4.0 x 10(14) mol 1(-1) Pu solutions of pH 3, 4 and 5. SEM observations showed that the accumulated Pu is evenly distributed on the upper and lower surfaces of P. tinctorum, in contrast to U(VI), which accumulated in both cortical and medullary layers. UV/VIS absorption spectroscopy demonstrates that a fraction of Pu(VI) in the solution is reduced to Pu(V) by the organic substances released from P. tinctorum, and the accumulated Pu on the surface is reduced to Pu(IV), while U(VI) keeps the oxidation state of VI. Since the solubility of Pu(IV) hydroxides is very low, reduced Pu(VI) does not penetrate to the medullary layers, but is probably precipitated as Pu(IV) hydroxides on the cortical lichen surface. It is concluded that the uptake and reduction of Pu(VI) by lichens is important to determine the mobilization and oxidation states of Pu in the terrestrial environment.     

Using sequential extraction techniques to assess the partitioning of plutonium and neptunium-237 from multiple sources in sediments from the Ob River (Siberia)

Sequential extraction techniques have been developed to assess partitioning of anthropogenic radionuclides (²⁴⁰Pu, ²³⁹Pu, and ²³⁷Np), originating from a variety of sources, as identified by using bulk sediment isotopic composition. Sediments were leached sequentially with a series of six chemical treatments designed to approximate different environmental processes that may occur or to selectively extract trace metals contained in different solid phases of the sediments (i.e., exchangeable, reducible, carbonate, organic, acid leachable, and refractory). Results indicate the majority of Pu and Np is similarly distributed within many of the extracted fractions, with the largest percentage (66–97%) of both elements being observed in sediments treated with buffered citrate dithionite (CDB), which targets easily reduced constituents such as Mn and Fe hydrous oxides. While these results do indicate an association of Pu and Np with redox sensitive elements, the environmental implications are unclear given that the CDB treatment is more extreme than naturally occurring conditions. Minor amounts of Np partition differently from Pu in sediments. The NH₄-acetate treatment, which is designed to liberate trace metals that are loosely adsorbed onto the surfaces of sedimentary materials such as hydrated iron oxides and humic substances, or present at exchangeable sites in clay minerals, mobilized ∼12% of the total Np while Pu levels were below detection. The H₂O₂ treatment, which is designed to liberate trace metals bound to organic matter, mobilized ∼8 and ∼1% of Np and Pu, respectively. These results indicate that a minor portion of the total Np may be affected by environmental conditions that have little or no effect on Pu. Between 7 and 24% of the Pu was observed in treatments designed to liberate Pu and Np that are tightly bound to lithogenic phases or refractory silicates. The ²⁴⁰Pu/²³⁹Pu observed in accessible and refractory fractions ranged between 0.11 and 0.18. With the exception of one sample, the ²⁴⁰Pu/²³⁹Pu isotope ratios measured in the refractory fractions are essentially identical having a mean ratio value of 0.123 ± 0.001 (1σ). The ²⁴⁰Pu/²³⁹Pu ratios provide isotopic evidence that suggests a portion of non-fallout contamination has a refractory nature. The presence of similarly low ²⁴⁰Pu/²³⁹Pu ratios in refractory fractions of sediments from the Ob and Irtysh Rivers suggests the existence of a source of refractory Pu which is consistent with refractory “hot particles” derived from surface tests at the Semipalitinsk test site.     

浅水湖泊孢粉和植物残体对水生植被的表现率

研究浅水湖泊中植物残体对水生植物的表现率,用于重建近代水生植被历史,可为治理湖泊富营养化,恢复湖泊生态环境提供依据。研究选址为英国北部的一个小湖泊,通过水生植物调查及表层沉积物中植物残体和孢粉分析,及地理信息系统方法定量研究植物残体对水生植物的表现率。结果表明：沉积物中植物残体精确地反映了植物优势种的存在;植物和植物残体的关系是很复杂的,有些植物在残体中表现率明显超高,而有些表现率偏低; 应把叶子和其它非繁殖植株部分作为恢复近代多年生植物历史依据;植物残体传输性较差,主要集中在植物母体附近;利用植物残体与孢粉分析相结合的方法能更准确地重建植被历史。     

Soil availability,plant uptake and soil to plant transfer of 99Tc--a review

The fission yield of 99Tc from 239Pu and 235U is similar to that of 137Cs or 90Sr and it is therefore an important component of nuclear weapons fall-out, nuclear waste and releases from nuclear facilities. There is particular current interest in 99Tc transfer from soil to plants for: (a) environmental impact assessments for terrestrial nuclear waste repositories, and (b) assessments of the potential for phytoextraction of radionuclides from contaminated effluent and soil. Vascular plants have a high 99Tc uptake capacity, a strong tendency to transport it to shoot material and accumulate it in vegetative rather than reproductive structures. The mechanisms that control 99Tc entry to plants have not been identified and there has been little discussion of the potential for phytoextraction of 99Tc contaminated effluents or soil. Here we review soil availability, plant uptake mechanisms and soil to plant transfer of 99Tc in the light of recent advances in soil science, plant molecular biology and phytoextraction technologies. We conclude that 99Tc might not be highly available in the long term from up to 50% of soils worldwide, and that no single mechanism that might be easily targeted by recombinant DNA technologies controls 99Tc uptake by plants. Overall, we suggest that Tc might be less available in terrestrial ecosystems than is often assumed but that nevertheless the potential of phytoextraction as a decontamination strategy is probably greater for 99Tc than for any other nuclide of radioecological interest.     

Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.     

Uranium uptake by hydroponically cultivated crop plants

Hydroponicaly cultivated plants were grown on medium containing uranium. The appropriate concentrations of uranium for the experiments were selected on the basis of a standard ecotoxicity test. The most sensitive plant species was determined to be Lactuca sativa with an EC₅₀ value about 0.1 mM. Cucumis sativa represented the most resistant plant to uranium (EC₅₀ = 0.71 mM). Therefore, we used the uranium in a concentration range from 0.1 to 1 mM.Twenty different plant species were tested in hydroponic solution supplemented by 0.1 mM or 0.5 mM uranium concentration. The uranium accumulation of these plants varied from 0.16 mg/g DW to 0.011 mg/g DW. The highest uranium uptake was determined for Zea mays and the lowest for Arabidopsis thaliana. The amount of accumulated uranium was strongly influenced by uranium concentration in the cultivation medium. Autoradiography showed that uranium is mainly localized in the root system of the plants tested. Additional experiments demonstrated the possibility of influencing the uranium uptake from the cultivation medium by amendments. Tartaric acid was able to increase uranium uptake by Brassica oleracea and Sinapis alba up to 2.8 times or 1.9 times, respectively. Phosphate deficiency increased uranium uptake up to 4.5 times or 3.9 times, respectively, by Brassica oleracea and S. alba. In the case of deficiency of iron or presence of cadmium ions we did not find any increase in uranium accumulation.     

Size-fractionated plutonium isotopes in a coastal environment

We have examined the distribution of individual Pu isotopes (239Pu, 240Pu, and 241Pu) in seawater from the Gulf of Maine (GOM). Samples were size-fractionated with a 1 kD cross-flow ultrafiltration (CFF) membrane. Subfractioned samples were radiochemically purified and Pu isotopes were analyzed using a three-stage thermal ionization mass spectrometer (TIMS). To our knowledge, this is the first time that both size class and Pu isotopic data have been obtained for seawater samples. Within measurement uncertainties a single 240Pu/239Pu atom ratio of 0.18 was found for all sample collection depths and sample size fractions. This signifies a current, single Pu source in GOM waters, namely global fallout, and suggests that no measurable isotopic fractionation occurred during CFF processing. The majority of Pu was found in the low molecular weight fraction (< 1 kD). Colloidal Pu varied from 8% of the total in surface waters to < 1% in the deepest (250 m) seawater sample. Evidence suggests that the vertical distribution of Pu in GOM is primarily controlled by conservative mixing processes. The high Pu fraction found in the low molecular size fraction implies that most of the Pu is in the non-particle-reactive oxidized fraction, and is consistent with the conservative Pu behavior. The activity levels are in agreement with other studies which show a slow decrease in Pu with time due to continued mixing and relatively slow particle removal.     

Plant uptake of neptunium-237 and technetium-99 under field conditions

Plant uptake of ⁹⁹Tc freshly added to soils was compared with uptake of ⁹⁹Tc ‘aged’ in soil for more than a decade. A combination of alkaline soil and freshly added ⁹⁹Tc resulted in elevated uptake into radish foliage (plant/soil concentration ratios ranged from 37 to 46). Neptunium-237 was freshly added to all soils. Neptunium uptake via plant roots into foliage was strongly affected by soil pH. Neptunium uptake was greatest from acidic soils. The observed plant/soil concentration ratios for ²³⁷Np under field conditions were approximately 10⁻² from acidic soils (pH 5·6–5·7) and were comparable to field concentration ratios for ²³⁹Pu, that is 10⁻³, from a basic soil (pH 7·5).     

Distribution and migration of 95Zr in a tea plant/soil system

(95)Zr is a primary radionuclide in the radioactive liquid efflux from a pressurized water reactor and one of the main radionuclides released after nuclear accidents. The fission yield of (95)Zr is as high as 6.2%, however, its environmental behavior has not been well documented. An experiment was conducted to evaluate the accumulation and distribution of (95)Zr in a tea plant/soil system. (95)Zr was accumulated primarily in the trunk of tea plants after being taken up from the soil. The radioactivity concentration of (95)Zr in the trunk increased slowly with time, then it reached a dynamic equilibrium 14 days after application. The radioactivity concentration of (95)Zr in the other parts of the tea plant was very low; only slighter greater than the detection limit. The results indicated that (95)Zr was not readily translocated in the tea plant. About 98.9% of applied (95)Zr was found to concentrate in the upper 5 cm layer after being sprayed onto the soil surface. The results indicated that (95)Zr could not readily move downwards with percolating water due to strong adsorption to surface soil.     

Assessing the fate of radioactive nickel in cultivated soil cores

Parameters regarding fate of ⁶³Ni in the soil–plant system (soil: solution distribution coefficient, K_d and soil plant concentration ratio, CR) are mostly determined in controlled pot experiments or from simple models involving a limited set of soil parameters. However, as migration of pollutants in soil is strongly linked to the water migration, variation of soil structure in the field and seasonal variation of evapotranspiration will affect these two parameters. The aim of this work was to explore to what extent the downward transfer of ⁶³Ni and its uptake by plants from surface-contaminated undisturbed soil cores under cultivation can be explained by isotopic dilution of this radionuclide in the pool of stable Ni of soils. Undisturbed soil cores (50 cm × 50 cm) were sampled from a brown rendzina (Rendzic Leptosol), a colluvial brown soil (Fluvic Cambisol) and an acidic brown soil (Dystric Cambisol) using PVC lysimeter tubes (three lysimeters sampled per soil type). Each core was equipped with a leachate collector. Cores were placed in a greenhouse and maize (DEA, Pioneer^®) was sown. After 44 days, an irrigation was simulated at the core surfaces to supply 10 000 Bq ⁶³NiCl₂. Maize was harvested 135 days after ⁶³Ni input and radioactivity determined in both vegetal and water samples. Effective uptake of ⁶³Ni by maize was calculated for leaves and kernels. Water drainage and leaching of ⁶³Ni were monitored over the course of the experiment. Values of K_d in surface soil samples were calculated from measured parameters of isotopic exchange kinetics. Results confirmed that ⁶³Ni was strongly retained at the soil surface. Prediction of the ⁶³Ni downward transfer could not be reliably assessed using the K_d values, since the soil structure, which controls local water fluxes, also affected both water and Ni transport. In terms of ⁶³Ni plant uptake, the effective uptake in undisturbed soil cores is controlled by isotope dilution as previously shown at the pot experiment scale.     

Uptake and depuration of 131I by the edible periwinkle Littorina littorea: uptake from seawater

Uptake and depuration experiments for the edible periwinkle Littorina littorea have been performed using 131I-labelled seawater. Throughout the experimental phase the winkles were fed on unlabelled Chondrus crispus. 131I concentrations in winkles during uptake followed linear first-order kinetics with an uptake half-time of 11 days, whereas for depuration a triphasic sequence with biological half-lives of 4, 23 and 56 days was determined. In general, iodine turnover in winkles via labelled seawater appears to be slower than observed for other molluscs (2-3 days). Most of the activity prior to and after depuration is found to be in the shell, with indications that shell and soft parts accumulate and depurate 131I at a similar rate. The operculum displays the highest specific activity of all fractions with a concentration factor of 750 l kg(-1). Concentration factors for whole winkle, shell, soft parts and digestive gland are in the order of 40-60 l kg(-1), higher than the IAEA recommended CF value for iodine in molluscs of 10 l kg(-1). The 131I CF in winkles is closer to that of the conservative radionuclides 99Tc and 137Cs than the CF of the particle reactive radionuclides (239,240)Pu and 241Am.     

The transfer of 239/240Pu to cow milk

In summer 1993 we measured the transfer of (239/240)Pu to milk from herbage from a pasture located 5 km from the Chernobyl nuclear power plant. In one treatment cows were allowed to graze freely on the pasture. In a second treatment, cows were fed herbage collected from the pasture in stalls. The milk transfer coefficient; F(m) did not vary significantly between treatments and the mean value of 7.5x10(-6)d l(-1) was higher than previously reported values. Despite many values of F(m) for Pu in the literature we identified few relevant original data sets. Transfer coefficient values for Pu are only appropriate when used in conjunction with a specified time period or an appropriate model which allows for the biological half-life. We recommend for screening purposes an F(m) value of 1x10(-5)d l(-1) for Pu, with an order of magnitude lower value being appropriate for cows which are only exposed for one grazing season.     

Particle and solution phase depth distributions of transuranics and 55Fe in the North Pacific

In situ large volume filtration and chemisorption techniques were used to collect samples from the North Pacific for radiochemical analyses of fallout transuranics and ⁵⁵Fe in filterable and filtered phases. The data cover several locations for surface collections and a detailed depth profile north of Hawaii at 30°N. The observed partition of these nuclides between suspended particulate and filtered phases is directly linked to the rates at which they are moved downward through the water column in association with sinking particles. Particulate phases in open ocean surface waters contain higher Pu (12–35%) than subsurface particulates (which average about 6%). ²⁴¹Am was found to exhibit much stronger particle association—typically close to 50% in both surface and subsurface waters—in accord with its known greater particle reactivity. In the high Pu deep water layer, particle associated Pu dropped to close to 1% of total Pu concentration. Together with a correlated increase in the proportion of oxidized Pu in this layer close to the sediment-water interface, this is taken as clear evidence of remobilization Pu from particles at, or near to, the interface. ⁵⁵Fe distributions on filtered particulates indicate a much deeper depth distribution relative to the transuranics. This may reflect both a higher particle association reactivity in respect to scavenging and a longer exposure history to scavenging (especially relative to ²⁴¹Am—produced by in situ decay).     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

The accumulation of plutonium by the edible winkle (Littorina littorea L.)

Laboratory experiments were carried out to measure the accumulation of ²³⁷Pu by the edible winkle from labelled sea water, food (seaweed), and silt. The equilibrium whole body concentration factor for ²³⁷Pu accumulation from sea water at 10°C was estimated as 34 with a biological half-time of 9 d. After 50 d accumulation, 83% of the measured whole body activity was present on the shell. In the flesh, the major sites for accumulation were the head/foot complex and the digestive gland. Depuration was found to be biphasic with components having half-times of 10 and 193 d respectively. Pu loss, following uptake from labelled Fucus spiralis, was biphasic with half-times of 1 and 69 d for the two components. Assimilation efficiency was tentatively estimated as 7%. Pu accumulation from labelled silt was low with an estimated transfer factor of 0.004; Pu loss was biphasic, with half-times similar to those for the seaweed experiment. Comparison of the laboratory-derived results with those for winkles from the environment showed that the food pathway was the main route for Pu accumulation, with the ingestion of silt playing a critical role in determining the final flesh Pu burden.     

The plant/soil concentration ratio for calcium,radium, lead,and polonium: Evidence for non-linearity with reference to substrate concentration

Evidence exists from both the literature and our own observations that plant nuclide uptake for a variety of plants and elements is a non-linear function of substrate concentration. The uptake response to increasing substrate concentration is usually in the form of a single or multi-phasic saturation curve. For some plant types and elements the uptake response may also take the form in which a threshold of soil activity is necessary before uptake is measurable. We present a generic uptake response curve and the resulting concentration ratio function determined by computer simulation. Data describing the uptake response of plants to ²²⁶Ra, ²¹⁰Pb and ²¹⁰Po as well as for calcium and stable lead are discussed. Functions are also presented for these elements to describe the uptake response and the concentration ratio and their mathematical forms are compared to the generic model.