Sellafield waste radionuclides in Irish sea intertidal and salt marsh sediments

Low level liquid radioactive waste discharges from the Sellafield nuclear fuel reprocessing plant in north west England had generated environmental inventories of about 3 × 10¹⁶ Bq of¹³⁷Cs, 6.8 × 10¹⁴ Bq of^239,240Pu and 8.9 × 10¹⁴ Bq of²⁴¹Am by 1990. Most of the^239,240Pu and²⁴¹Am and about 10% of the¹³⁷Cs has been retained in a deposit of fine marine sediment close to the discharge point. The quantities of radionuclides discharged annually from Sellafield decreased by two orders of magnitude from the mid-1970s to 1990 but estimated critical group internal and external exposure decreased by less than one order of magnitude over this period. This indicates that during the period of reduced discharges, radionuclides already in the environment from previous releases continued to contribute to the critical group exposure and highlights the need to understand processes controlling the environmental distribution of the radionuclides. Redistribution of the contaminated marine sediment is potentially of major significance in this context, in particular if it results in transport of radionuclides to intertidal areas, where contact with the human population is relatively likely. A review is presented of published work relating to Sellafield waste radionuclides in Irish Sea sediments. Data on temporal and spatial trends in radionuclide concentrations and activity ratios are collated from a number of sources to show that the dominant mechanism of radionuclide supply to intertidal areas is by redistribution of the contaminated marine sediment. The implications of this mechanism of supply for trends in critical group radiation exposure are considered.     

Temperature effects on accumulation and retention of radionuclides in the sea star,Asterias forbesi: implications for contaminated northern waters

Radioactive waste disposal and nuclear testing concentrated in high latitudes in the northern hemisphere have resulted in the accumulation of radionuclides in Arctic marine ecosystems, but little is known of the consequences for marine biota in these waters. Under controlled laboratory conditions in May through September 1994, we examined the bioaccumulation in sea stars, Asterias forbesi (Desor), or the radionuclides ²⁴¹Am, ⁵⁷Co and ¹³⁷Cs, all of which are important components of disposed radioactive wastes. Experiments at 2 and 12°C determined the relative importance of food (the bivalve, Macoma balthica) and water as sources of radionuclides and assessed the influence of temperature on radionuclide influx and efflux rates. The lower temperature greatly increased the retention of radionuclides ingested with food; for instance, the biological half-life (tb _1/2) of ²⁴¹Am in the sea stars was 31 d at 12°C, but was virtually infinite at 2°C. Retention of ingested ⁵⁷Co was also increased at 2°C (tb _1/2=41 d). ¹³⁷Cs was not accumulated from food. Low temperature significantly reduced net influx rates of ¹³⁷Cs from water, but did not affect net uptake of ²⁴¹Am or ⁵⁷Co. Temperature had little effect on the retention of all three isotopes obtained from the dissolved phase. These experiments suggest that extrapolation of results of previous radioecological studies, conducted at warmer temperatures, to polar or temperate winter environments may be problematic, and that nuclear waste isotopes obtained through trophic transfer may be retained far more efficiently in high latitude marine biota than by fauna from warmer ecosystems.     

Horizontal Distribution of Some Artificial Radionuclides in Sediments Collected Off the Rhone Mouth (Gulf of Lions-Mediterranean Sea)

Abstract

The Rhône delta is a typical microtidal estuary. River runoff spreads out into the Gulf of Lions as a surface plume influenced by the prevailing N or NW wind and the Liguro-Provençal-Catalan current. in the prodelta, sediments form a filter that traps radionuclides released by the different nuclear installations on the Rhône River and which are associated with fine particles. the horizontal distribution of various artificial radionuclides shows the highest concentrations at the Rhône River mouth. There,¹³⁷Cs reaches 86.6 and 94.4 Bq·kg^?1 dry wt. and is still present 10 miles away (32.5 Bq·kg^?1 dry wt.) in the southwestward direction (influence of the general circulation). Data obtained in the sediment at Roustan station between 1980 and 1990 show that in 1990, ¹³⁷Cs levels were similar to those found previous to the Chernobyl accident.     

Transport and redistribution of Chernobyl fallout radionuclides by fluvial processes: Some preliminary evidence

Several measurements of¹³⁷Cs concentrations in suspended sediment transported by the River Severn during the post-Chernobyl period and in recent channel and floodplain deposits along the river emphasise the potential significance of fluvial processes in the transport and concentration of fallout radionuclides.     

Sediment accumulation and bio-diffusion mixing rates derived from excess <Superscript>210</Superscript>Pb and <Superscript>137</Superscript>Cs profiles in sediment cores of Mumbai Harbor Bay

Bio-diffusion mixing rates (D_b) were estimated from depth profiles of excess ²¹⁰Pb and ¹³⁷Cs in three sediment cores collected from Mumbai Harbour Bay (MHB) using a steady state vertical advection - diffusion model. The mean of ²¹⁰Pb and ¹³⁷Cs derived D_b values along the studied area were obtained to be about 23 and 36 cm²y^?1 respectively. These derived values were within the range of literature values reported for other equivalent environment internationally. The relatively higher D_b values for ¹³⁷Cs profiles demonstrated that particles have diffused more intensely within the surface layer of sediments over 1 year. Conversely, low D_b values for ²¹⁰Pb indicate slow mixing rates in the sediment profile which might be resulted from low ²¹⁰Pb flux and diffusion of ²²²Rn to the seafloor. The significant differences between ²¹⁰Pb and ¹³⁷Cs derived D_b values among cores indicate that there appeared to be as regional differences in sediment properties and local variability in the intensity of seafloor mixing. Furthermore, D_b values also depend on differences in characteristic time and depth scales of radionuclides in cores, benthic fauna abundances, organic carbon flux to the sediments and primary production in overlying surface waters. Comparison of ²¹⁰Pb derived D_b values with those calculated from ¹³⁷Cs distributions reveals better agreement for core 2 than core 1 and 3. The agreement may be fortuitous because ¹³⁷Cs appears significantly deeper than ²¹⁰Pb in all cores. It was also observed that D_b values increases as sediment accumulation rate increases for both radionuclide.     

Environmental risk assessment of radioactivity and heavy metals in soil of Toplica region,South Serbia

Activity levels of natural and artificial radionuclides and content of ten heavy metals (As, Cd, Co, Cr, Cu, Mn, Ni, Pb, Zn and Hg) were investigated in 41 soil samples collected from Toplica region located in the south part of Serbia. Radioactivity was determined by gamma spectrometry using HPGe detector. The obtained mean activity concentrations ± standard deviations of radionuclides ²²⁶Ra, ²³²Th, ⁴⁰K and ¹³⁷Cs were 29.9 ± 9.4, 36.6 ± 11.5, 492 ± 181 and 13.4 ± 18.7 Bq kg⁻¹, respectively. According to Shapiro–Wilk normality test, activity concentrations of ²²⁶Ra and ²³²Th were consistent with normal distribution. External exposure from radioactivity was estimated through dose and radiation risk assessments. Concentrations of heavy metals were measured by using ICP-OES, and their health risks were then determined. Enrichment by heavy metals and pollution level in soils were evaluated using the enrichment factor, the geoaccumulation index (I_geo), pollution index and pollution load index. Based on GIS approach, the spatial distribution maps of radionuclides and heavy metal contents were made. Spearman correlation coefficient was used for correlation analysis between radionuclide activity concentrations and heavy metal contents.

     

Release,deposition and elimination of radiocesium (137Cs) in the terrestrial environment

Radionuclide contamination in terrestrial ecosystems has reached a dangerous level. The major artificial radionuclide present in the environment is ¹³⁷Cs, which is released as a result of weapon production related to atomic projects, accidental explosions of nuclear power plants and other sources, such as reactors, evaporation ponds, liquid storage tanks, and burial grounds. The release of potentially hazardous radionuclides (radiocesium) in recent years has provided the opportunity to conduct multidisciplinary studies on their fate and transport. Radiocesium’s high fission yield and ease of detection made it a prime candidate for early radio-ecological investigations. The facility setting provides a diverse background for the improved understanding of various factors that contribute toward the fate and transfer of radionuclides in the terrestrial ecosystem. In this review, we summarize the significant environmental radiocesium transfer factors to determine the damaging effects of radiocesium on terrestrial ecosystem. It has been found that ¹³⁷Cs can trace the transport of other radionuclides that have a high affinity for binding to soil particles (silts and clays). Possible remedial methods are also discussed for contaminated terrestrial systems. This review will serve as a guideline for future studies of the fate and transport of ¹³⁷Cs in terrestrial environments in the wake of the Fukushima Nuclear Power Plant disaster in 2011.     

Geochemical Associations of Sellafield-Derived Radionuclides in Saltmarsh Deposits of the Solway Firth

This paper describes a study of the geochemical associations of Sellafield waste radionuclides in saltmarsh sediments from south-west s]Scotland. The contaminant radionuclides are transported to this environment in association with particulate material and ¹³⁷Cs was found to be predominantly (80-98%) non-extractable. In the case of ^239+240Pu there was a redistribution from the oxalate extractable oxide fraction to the pyrophosphate extractable organic fraction as a consequence of on-shore transfer of contaminated sediment. The relatively aggressive nature of the chemical extractants required to remove the radionuclides from the sediments suggests that they were in a form which was unlikely to result in their being released into the aquatic environment or taken up by plants. Plutonium had a greater potential mobility or bioavailability than Cs. Values of K^D for the desorption of ¹³⁷Cs from the sediment by freshwater, groundwater and seawater were all approximately 10⁵ L kg^-1, confirming its immobility in this environment. The desorption K_D values for stable ¹³³Cs were all approximately 10⁶ L kg^-1, so the stable Cs did not have a significant influence on the radiocaesium in this sediment.     

Etude de la décontamination d'Arenicola marina (annélide,polychète) après contamination expérimentale par le caesium 137 ou le cobalt 60

From a nuclear protection standpoint, problems of decontamination are of great interest. In Arenicola marina L. a comparative study has been made on the elimination of two radionuclides, the metabolic functions of which are very different: ¹³⁷Cs and ⁶⁰Co. After experimental contamination with ¹³⁷Cs, significant decontamination is possible; however, elimination of ¹³⁷Cs accumulated in muscles is very slow. The elimination of ⁶⁰Co is very slow; its biological half-life in A. marina is about 3 months.     

137 Cs在我国滨海核电周边海洋生物的富集及生态风险研究

铯-137(~(137)Cs)是滨海核电站液态流出物中主要人工放射性核素和重要监控指标之一,易被水生生物累积,有关核电周边海域内海洋生物的核素富集状况备受关注。通过分析海洋生物富集放射性~(137)Cs的方式、生物富集系数的种群特征、人工放射性核素在生物体内的辐射剂量率状况,结果显示:1)滨海核电周边海域内~(137)Cs的放射性水平较低; 2)海洋生物对于~(137)Cs的富集未呈现显著的种群规律; 3)目前对放射性铯的富集能力较高的生物主要是底栖生物; 4)核电厂周边海域内海洋生物通常未达到可导致电离辐射损伤的辐射剂量率水平。随着滨海核电在我国的大力发展,对能够快速反映环境放射性状况的指示生物的筛选、生物放射性质量安全及其生态健康风险需进一步关注。     

Radioaktive Isotope in Sedimenten

The Federal Office for Radiation Protection investigated several natural and artificial radioactive isotopes in the sediments of rivers in the Erzgebirge by means of gamma radiation spectrometry. The regional distribution of the isotopes and their relation to former uranium mining is described. The significantly high differences of their concentrations in different river sections are discussed. A dependence of the activity concentrations on temporal peaks in mining activities is illustrated by the example of a sediment profile. The behavior of artificial radioactive isotopes, such as¹³⁷Cs and¹³⁴Cs after the reactor accident in Tschernobyl is characterized. All measurements were evaluated from the radiological point of view and critically assessed.     

Inventories and Distribution of Radiocaesium in Arctic Marine Sediments: Influence of Biological and Physical Processes

Abstract

Extensive surveys of sediment burdens of radiocaesium, specifically ¹³⁷Cs, and other radioactive contaminants in the Arctic during the 1990′s, indicate that almost all anthropogenic radionuclides buried on continental shelves adjacent to Alaska are derived from global bomb fallout. the ¹³⁷Cs (half-life: 30.2y) activities observed in surface (0–4 cm) marine sediments however, vary widely, albeit much less than the expected current inventory resulting from bomb fallout at this latitude (～100mBq cm^?2). This observed geographical variation provided the opportunity to evaluate physical and biological mechanisms that may affect caesium biogeochemistry on Arctic continental shelves. We investigated whether high biological productivity in portions of the Bering and Chukchi Seas is effective in removing dissolved radiocaesium from the water column, and whether biological production in overlying water affects total radiocaesium inventories in sediments. Based upon C/N ratios in the organic fraction of shallow sediments, we found no evidence that higher inventories or surface activities of radiocaesium are present in areas with higher deposition of particulate organic matter. Based upon stable carbon isotope ratios of organic matter in sediments, we found no evidence that terrestrial runoff contributes proportionally to higher surface activities, although terrestrial runoff may affect total inventories of the radionuclide. Radiocaesium content of surface sediments was significantly correlated with total organic carbon content of sediments and the proportion of sediments in the finest sediment fractions. Because high current flow can also be expected to influence distributions of those sedimentary parameters, we conclude that re-distribution of     

Sediment environmental capacity of 137Cs in Daya Bay

Sediment environmental capacity of pollutants is very important for marine environmental management. Based on the methodology of a study on water, soil environmental capacity, and mass conservation theory in a system, the concept and model on sediment environmental capacity for ¹³⁷Cs in Daya Bay were developed. The static capacity for ¹³⁷Cs in the upper sediment near the shore at a shallow area was calculated, and the annual dynamic capacity and total dynamic capacity were also calculated through determination of the typical biomass in the sediment. The results showed that the estimated environmental capacity for ¹³⁷Cs in sediments was approximately equal to the current input of ¹³⁷Cs into the sediments. Controlling the input of ¹³⁷Cs in the sediments within the environmental capacity guarantees the sustainability of the current situation of the Daya Bay ecosystem and avoidance of a significant degradation of the system.     

河流放射性核素水体弥散模型及其应用

随着我国核能及核技术利用产业的迅速发展,放射性物质运输对饮用水水源地的潜在放射性污染健康风险越来越大,阐明事故情况下放射性物质在地表水体中的迁移弥散行为可为居民饮水健康风险防范提供科学依据。针对含钴-60、铯-137、锶-90货包公路运输在事故工况下放射性物质释放造成黄河兰州段河流型饮用水源放射性污染,讨论了河流放射性物质弥散模型和居民饮用水的健康风险。结合国内现有放射源活度水平及国内外放射性物质事故资料,考虑泥沙的影响,设定铯-137不同活度水平、不同流量情形,根据饮用水中铯-137的死亡风险系数和患病风险系数对距离事故点为64 km、114 km的河流下游两个饮用水源地居民饮用受污染自来水存在的健康风险进行评估,同时选择钴-60、锶-90两种核素以30年间河水平均流量偏小值为例进行对比评估。放射性核素在黄河河流的稀释作用下,由饮用受钴-60、铯-137、锶-90污染的水随放射源活度、河水流量及泥沙含量的变化存在不同程度的死亡风险与患病风险。因此,应当对受到放射性污染的水源及时采取适当措施,预防放射性核素造成的风险。     

Retention of 137cesium in acid sulphate soils of South Central Thailand

Adsorption and desorption of ¹³⁷Cs by acid sulphate soils from the Nakhon Nayok province, South Central Plain of Thailand located near the Ongkarak Nuclear Research Center (ONRC) were investigated using a batch equilibration technique. The influence of added limestone (12 and 18 tons ha^?1) on ¹³⁷Cs adsorption–desorption was studied. Based on Freundlich isotherms, both adsorption and desorption of ¹³⁷Cs were nonlinear. A large portion (98.26–99.97%) of added ¹³⁷Cs (3.7?×?10³?7.03?×?10⁵ Bq l^?1) was sorbed by the soils with or without added lime. The higher lime treatments, however, favoured stronger adsorption of ¹³⁷Cs as compared with soil with no lime, which was supported by higher K _ads values. The addition of lime, the cation exchange capacity and pH of the soil increased and hence favoured the stronger adsorption of ¹³⁷Cs. Acid sulphate soils with a high clay content, medium to high organic matter, high CEC, and predominant clay types consisting of a mixture of illite, kaolinite, and montmorillonite were the main soil factors contributing to the high ¹³⁷Cs adsorption capacity. Competing cations such as NH₄ ⁺, K⁺, Na⁺, Ca²⁺, and Mg²⁺ had little influence on ¹³⁷Cs adsorption as compared with liming, where a significant positive correlation between K _ads and soil pH was observed. The ¹³⁷Cs adsorption–desorption characteristics of the acid sulphate soils studied exhibited a very strong irreversible sorption pattern. Only a small portion (0.09–0.58%) of ¹³⁷Cs adsorbed at the highest added initial ¹³⁷Cs concentration was desorbed by four successive soil extractions. Results clearly demonstrated that Nakhon Nayok province acid sulphate soils have a high ¹³⁷Cs adsorption capacity, which limits the ¹³⁷Cs bioavailability.     

Biokinetics of plutonium,americium and californium in the marine isopod Cirolana borealis,with observations on its feeding and molting behavior

In a series of laboratory experiments carried out during 1982, the biokinetics of ²³⁷Pu (IV), ²³⁷Pu (V), ²⁴¹Am (III), and ²⁵²Cf (III) were studied in the benthic marine isopod Cirolana borealis Lilljeb. Following a 3 wk exposure to labelled seawater, isopods reached non-equilibrium concentration factors of 52±15, 54±12, 176±14, and 185±53 for Pu (IV), Pu (V), Am and Cf, respectively. Uptake of these radionuclides occurred to a great extent by surface adsorption, with the major fraction of the accumulated radionuclides being associated with exoskeleton and lesser percentages located in gut, digestive gland, muscle and haemolymph. The pattern of radiotracer depuration was in all cases biphasic, with the long-lived retention compartment retaining the largest fraction of whole-body radioactivity. Biological half-lives for radionuclide turnover in the long-lived compartment were 60±3 d, 87±5 d, 261±12 d and 288±60 d for Pu (IV), Pu (V), Am and Cf, respectively. Examination of radionuclide distribution among tissues following longterm depuration showed that the radionuclides were eliminated from internal tissues more rapidly than from the exoskeleton. Uptake and depuration studies indicated that the biokinetics of americium and californium were similar to each other, but that they differed significantly from those of oxidized and reduced plutonium. In general, these experimental results support previous reports that americium and californium are more bioavailable than plutonium in the marine waters. The fraction americium and californium assimilated into tissue from food was very low and did not exceed 5%. Unassimilated labelled food was often retained in the gut for more than 2 mo and released only infrequently in a loosely bound condition. In the event of contamination, this particular feeding-digestion strategy in highly mobile, scavenging isopods could act as a potential biological mechanism for the widespread dispersion of radioactive wastes.     

Assimilation,inter-organ transfer and excretion of americium in two teleost fish

Radiotracer experiments were performed (February–April, 1982) to study the assimilation and metabolism of the transuranium nuclide americium-241 in the marine teleosts Serranus scriba (Linnaeus, 1758) and Scorpaena notata Rafinesque, 1810, caught off the Monaco coast. Fish fed with ²⁴¹Am-labelled food showed that assimilation of this radionuclide takes place through the gastrointestinal walls and that the small fraction accumulated is incorporated mainly in the skin, muscle and skeleton. Gut-transfer coefficients were similar in both species and averaged 0.7% (range 0.1 to 1.7%) of the ingested activity. The calculated biological half-lives for loss of the absorbed fraction ranged between 49 and 61 d for Serranus scriba and 12 and 117 d for Scorpaena notata. Results from an intramuscular injection experiment indicated that ²⁴¹Am was retained mainly in the liver, skin and skeleton; the fraction accumulated by muscle was very low. Liver displayed a relatively short biological half-time for ²⁴¹Am loss of roughly 24 d. Routes of ²⁴¹Am excretion from the teleosts appear to be through the kidneys, gills and feces with bile serving as a possible excretion route from the liver. From the limited amount of published information available for comparison, experimental evidence is presented which suggests that ²⁴¹Am taken up via the food chain is more biologically available to marine fish than is plutonium.     

Seasonal variation of the concentrations of 137Cs in sediment,sea water,and some organisms collected from Izmir Bay and Didim

¹³⁷Cs in the marine environment mainly originates from fallout of atmospheric nuclear weapon tests, accidental releases from nuclear facilities, and from the Chernobyl accident. After the latter accident, many studies have been carried out in Turkey. The objective of this study is to assess the spatial distribution of ¹³⁷Cs in the coastal marine environment of the Aegean Sea.

The concentrations of ¹³⁷Cs in sediment, sea water, mussel (Mytilus galloprovincialis), and fish samples collected from the coast of the Aegean Sea at Izmir Bay and near Didim (Akbük) have been monitored for seasonal variability by the means of gamma spectroscopy: they vary between 0.10 ± 0.01 and 1.5 ± 0.3 Bq kg^?1, 1.3 ± 0.1 and 4.3 ± 0.4 Bq m^?3, <0.2 and 1.3 ± 0.3 Bq kg^?1, and 0.20 ± 0.03 and 1.8 ± 0.3 Bq kg^?1, respectively.     

Cs-137 contamination in forest ecosystems in southwest Rila Mountain, Bulgaria

We studied Cs-137 contamination and radionuclide transfer in mountain forest ecosystems from Bulgaria. Here we show the first analyses of Cs-137 soil-to-plant transfer and we assess that it depends on the soil organic matter content and the specifics of the tree species. The forest litter is strong polluted with Cs-137 and is a barrier for its migration. In the upper 0-5 cm of the soil the Cs content ranges from 52 to 81 Bq kg^–1 then decreases in deeper layers. The 1-year-old needles of spruce, fir, and Scots pine accumulate more cesium than the fine roots. The values of the needles transfer factor range between 0.3 and 0.58. The fine roots transfer factor varies between 0.1 and 0.32.     

Cäsium-137 in Böden saarländischer Waldökosysteme

Scopes and main features

In order to explain the behaviour of the artificial radioisotope¹³⁷Cs towards landscape resources in the Saar-Lor-Lux-Region, the cross-border region between southwestern Germany/ Saarland, France/Lorraine and Luxembourg, regional distribution as well as downward translocation and depth functions of¹³⁷Cs in the main soil substrates of forest ecosystems in the Saarland were investigated.

Results

The study shows that the highest¹³⁷Cs activities are found in the north of the Saarland, whereas the south and south-eastern regions show distinctly lower concentrations of¹³⁷Cs. Migration rates range between 0.25 cm/a and 1.0 cm/a. On an average, the highest migration rates were found in the clayey-silty substrates of the lime stone areas in theMuschelkalk regions (Middle Triassic) (0.66 cm/a), followed by the loamy substrates of Lower Permian clastic sediments (Unterrotliegendes) (0.53 cm/a) and the sandy substrates of theBuntsandstein areas (Lower Triassic sandstone) (0.41 cm/a). 90 to 95% of the¹³⁷Cs activities in the clay-poor soils of the Unterrotliegendes and the Buntsandstein were traced in the upper 10 cm of the humus topsoil. The substrates of the lime stone areas (Muschelkalk), in contrast to this, reveal a¹³⁷Cs activity of only 70–76% at the same depth.

Conclusions

Due to the fact that the primary and secondary pores of the soil pore system, in their function as translocation pathways, decrease with increasing soil depth, a significant reduction in the migration rates of¹³⁷Cs can be expected with increasing soil depth. On the other hand, the maximal migration depth of 40 cm found in shallow soils on jointed parent material, as well as on sites with high groundwater tables, implies a possible contamination of near-surface groundwater.

Future outlook

Based on the results of this study, a permanent monitoring of¹³⁷Cs was added to the long-term Soil Monitoring Program run by the Federal Administrative Office of Environment of the Saarland (Landesamt für Umweltschutz des Saarlandes)