Radionuclides in marine macroalgae from Amchitka and Kiska Islands in the Aleutians: establishing a baseline for future biomonitoring

Levels of radionuclides in seven species of marine brown algae and Ulva were determined to establish a baseline for the Northern Pacific Ocean/Bering Sea (Aleutian Islands). There were differences in levels among algal species and locations (Amchitka Island vs Kiska Island). No values were above the minimum detectable activity (MDA) level for (137)Cs, (129)I, (60)Co, (152)Eu, (90)Sr, and (99)Tc. There were interspecific differences in some radionuclides: Ulva lactuca (=Ulva fenestrata) had the highest levels of (241)Am, Alaria fistulosa had the highest levels of (239,240)Pu, and Fucus distichus (=Fucus gardneri) had the highest levels of (234)U, (235)U, and (238)U. However, levels of all radionuclides were generally low and near the MDA for all isotopes. Although Amchitka Island had higher levels of (239,240)Pu than Kiska, the differences were very small and not significant biologically. The data indicate that algae can be useful bioindicators of actinides because they accumulate them at very low environmental levels, allowing them to provide early warning of any potential seepage of radionuclides into the marine environment. Further, the data indicate that some species (the intertidal Fucus) are better accumulators than others, and these should be used as bioindicators in future monitoring schemes.     

Background exposure rates of terrestrial wildlife in England and Wales

It has been suggested that, when assessing radiation impacts on non-human biota, estimated dose rates due to anthropogenically released radionuclides should be put in context by comparison to dose rates from natural background radiation. In order to make these comparisons, we need data on the activity concentrations of naturally occurring radionuclides in environmental media and organisms of interest. This paper presents the results of a study to determine the exposure of terrestrial organisms in England and Wales to naturally occurring radionuclides, specifically (40)K, (238)U series and (232)Th series radionuclides. Whole-body activity concentrations for the reference animals and plants (RAPs) as proposed by the ICRP have been collated from literature review, data archives and a targeted sampling campaign. Data specifically for the proposed RAP are sparse. Soil activity concentrations have been derived from an extensive geochemical survey of the UK. Unweighted and weighted absorbed dose rates were estimated using the ERICA Tool. Mean total weighted whole-body absorbed dose rates estimated for the selected terrestrial organisms was in the range 6.9 x 10(-2) to 6.1 x 10(-1) microGy h(-1).     

Assessment of radiological effects on the regional environment due to the operation of the Tokai Reprocessing Plant

The regional environmental radiological effects were assessed for the past 25-year operation of the Tokai Reprocessing Plant (TRP). The assessment was basically performed with the environmental radiological monitoring data around the TRP. For the environmental monitoring, various kinds of terrestrial and marine samples including air dust, surface soil, polished rice grain, leafy vegetable, milk, seawater, seabed sediments, fish, shellfish and seaweed were collected in the surrounding environment of the TRP. Radionuclides such as (3)H, (14)C, (90)Sr, (137)Cs and (239,240)Pu in the environmental samples were determined by radiochemical methods. However, they showed no significant short-term increase or long-term accumulation of radionuclides discharged from the TRP. Therefore, the public dose was evaluated using the mathematical models and the discharge data of radionuclides. The estimated annual effective dose for the public was about 0.1% of the annual effective dose limit recommended by the ICRP. The assessment showed that there were no significant radiological effects on the environment and the public due to the 25-year operation of the TRP.     

Technetium-99 in the Irish marine environment

Technetium-99 activity concentrations in seawater and biota from Irish coastal waters are presented. Time series measurements of 99Tc in seawater and Fucus vesiculosus from the western Irish Sea show that activity concentrations have increased in line with the increase in discharges of 99Tc from Sellafield. The peak in activity concentrations in both seawater and Fucus vesiculosus occurred in 1997 approximately two years after the peak in 99Tc discharges. The highest activity concentration recorded in Fucus vesiculosus showed a 29-fold increase over the mean concentration for the period 1988-1993. Technetium-99 activity concentrations were measured in fish, lobsters, prawns, mussels and oysters landed at major fishing ports on the east and northeast coasts of Ireland between 1996 and 1998. Concentration factors for 99Tc in the brown seaweed Fucus vesiculosus and certain species of fish, crustaceans and molluscs from the Irish Sea were estimated. In general, these concentration factors were higher than those in the literature which were derived from laboratory studies, but agreed well with values which were based on field studies. The mean committed effective doses to Irish typical and heavy seafood consumers due to 99Tc in the period 1996-1998 were 0.061 and 0.24 microSv, respectively.     

A biomonitoring plan for assessing potential radionuclide exposure using Amchitka Island in the Aleutian chain of Alaska as a case study

With the ending of the Cold War, the US and other nations were faced with a legacy of nuclear wastes. For some sites where hazardous nuclear wastes will remain in place, methods must be developed to protect human health and the environment. Biomonitoring is one method of assessing the status and trends of potential radionuclide exposure from nuclear waste sites, and of providing the public with early warning of any potential harmful exposure. Amchitka Island (51 degrees N lat, 179 degrees E long) was the site of three underground nuclear tests from 1965 to 1971. Following a substantive study of radionuclide levels in biota from the marine environment around Amchitka and a reference site, we developed a suite of bioindicators (with suggested isotopes) that can serve as a model for other sites contaminated with radionuclides. Although the species selection was site-specific, the methods can provide a framework for other sites. We selected bioindicators using five criteria: (1) occurrence at all three test shots (and reference site), (2) receptor groups (subsistence foods, commercial species, and food chain nodes), (3) species groups (plants, invertebrates, fish, and birds), (4) trophic levels, and (5) an accumulator of one or several radionuclides. Our major objective was to identify bioindicators that could serve for both human health and the ecosystem, and were abundant enough to collect adjacent to the three test sites and at the reference site. Site-specific information on both biota availability and isotope levels was essential in the final selection of bioindicators. Actinides bioaccumulated in algae and invertebrates, while radiocesium accumulated in higher trophic level birds and fish. Thus, unlike biomonitoring schemes developed for heavy metals or other contaminants, top-level predators are not sufficient to evaluate potential radionuclide exposure at Amchitka. The process described in this paper resulted in the selection of Fucus, Alaria fistulosa, blue mussel (Mytilus trossulus), dolly varden (Salvelinus malma), black rockfish (Sebastes melanops), Pacific cod (Gadus macrocephalus), Pacific halibut (Hippoglossus stenolepis), and glaucous-winged gull (Larus glaucescens) as bioindicators. This combination of species included mainly subsistence foods, commercial fish, and nodes on different food chains.     

Radiological risk assessment and biosphere modelling for radioactive waste disposal in Switzerland

Long-term safety assessments for geological disposal of radioactive waste in Switzerland involve the demonstration that the annual radiation dose to humans due to the potential release of radionuclides from the waste repository into the biosphere will not exceed the regulatory limit of 0.1 mSv. Here, we describe the simple but robust approach used by Nagra (Swiss National Cooperative for the Disposal of Radioactive Waste) to quantify the dose to humans as a result to time-dependent release of radionuclides from the geosphere into the biosphere. The model calculates the concentrations of radionuclides in different terrestrial and aquatic compartments of the surface environment. The fluxes of water and solids within the environment are the drivers for the exchange of radionuclides between these compartments. The calculated radionuclide concentrations in the biosphere are then used to estimate the radiation doses to humans due to various exposure paths (e.g. ingestion of radionuclides via drinking water and food, inhalation of radionuclides, external irradiation from radionuclides in soils). In this paper we also discuss recent new achievements and planned future work.     

Distribution of gamma-ray emitting radionuclides in the environment of Burullus Lake: I. Soils and vegetations

The concentrations and distribution of gamma-ray emitting isotopes in Burullus Lake were investigated with the aim of evaluating the environmental radioactivity. Particularly in wetlands, natural properties of the environment can cause the actual inventory to be different from the activity originally deposited. The mean concentrations of (226)Ra, (232)Th and (40)K were 14.3, 15.5 and 224 Bq/kg, respectively, in the coastal soils. On the other hand, soil samples from the islands had mean concentrations of 13.5, 17.4 and 341 Bq/kg for (226)Ra, (232)Th and (40)K, respectively. Samples from coast and islands show evidence of possible transfer and accumulation of the (137)Cs radionuclide. The mean (137)Cs activity concentrations in the soil samples were 1.2 and 15.1 Bq/kg in the coast and islands, respectively. The vertical migration of (137)Cs was studied based on its content in the consequently located three soil layers down to 30 cm depth. The radium equivalent, dose rate in air and annual dose equivalent from the terrestrial natural gamma-radiation were evaluated. The mean activity concentrations of the gamma-ray emitting radionuclides in vegetation were relatively low.     

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.     

Derivation of a screening methodology for evaluating radiation dose to aquatic and terrestrial biota

The United States Department of Energy (DOE) currently has in place a radiation dose standard for the protection of aquatic animals, and is considering additional dose standards for terrestrial biota. These standards are: 10 mGy/d for aquatic animals, 10 mGy/d for terrestrial plants, and, 1 mGy/d for terrestrial animals. Guidance on suitable approaches to the implementation of these standards is needed. A screening methodology, developed through DOE's Biota Dose Assessment Committee (BDAC), serves as the principal element of DOE's graded approach for evaluating radiation doses to aquatic and terrestrial biota. Limiting concentrations of radionuclides in water, soil, and sediment were derived for 23 radionuclides. Four organism types (aquatic animals; riparian animals; terrestrial animals; and terrestrial plants) were selected as the basis for development of the screening method. Internal doses for each organism type were calculated as the product of contaminant concentration, bioaccumulation factor(s) and dose conversion factors. External doses were calculated based on the assumption of immersion of the organism in soil, sediment, or water. The assumptions and default parameters used provide for conservative screening values. The screening methodology within DOE's graded approach should prove useful in demonstrating compliance with biota dose limits and for conducting screening assessments of radioecological impact. It provides a needed evaluation tool that can be employed within a framework for protection of the environment.     

A probabilistic approach to obtaining limiting estimates of radionuclide concentration in biota

The US Department of Energy has developed a graded approach for evaluating radiation doses to biota. Limiting concentrations of radionuclides in water, soil, and sediment were derived for twenty-three radionuclides. Four organism types (aquatic animals, riparian animals, terrestrial animals, and terrestrial plants) were selected as the basis for method development. While environmental transfer data needed for deriving biota tissue concentrations are available for aquatic animals and terrestrial plants, less information is available for terrestrial and riparian organisms. Two methods were applied and examined for their ability to provide estimates of organism:soil or organism:water concentration factors in lieu of measured data. The kinetic/allometric approach combined with a parameter uncertainty analysis provides a needed method to estimate concentration factors across multiple species with limited input data.     

The presence of some artificial and natural radionuclides in a Eucalyptus forest in the south of Spain

Long-lived artificial radionuclides (137Cs, 90Sr) were studied in a Eucalyptus plantation located in the south-west of Spain. Radionuclide concentrations were determined in different types of samples corresponding to specific forest components (soil, trees, herbs and litter). Depth profile distributions were obtained in two selected core soils. Two layers were separately measured in three other cores. The concentration factor, defined as the ratio between the mean activity concentration in a component and the mean activity concentration in the soil, was calculated for each component. The biomass of different components was estimated in order to evaluate the total density concentration (Bq/ha) of the artificial radionuclides (137Cs, 90Sr) in the Eucalyptus plantation. The transfer of the radionuclides between the different forest components can be inferred from the results. Additionally, other naturally occurring radionuclides (40K, 226Ra, 228Ra, 228Ac) were determined for comparison. Transport of radionuclides from forest to a nearby pulp mill is also discussed.     

Radioactivity concentrations and dose assessment for soil samples around Adana, Turkey

The concentrations of natural radionuclides in surface soils around Adana, Turkey were determined using gamma ray spectrometry with an HPGe detector. The natural gamma ray radioactivity of the terrestrial radionuclides in air was calculated throughout different areas of Adana. The average activity concentrations of (238)U, (232)Th and (40)K were found to be 17.6, 21.1 and 297.5 Bq kg(-1), respectively. Outdoor gamma dose measurements in air 1m above ground level were determined by using a portable gamma scintillation detector. The gamma dose measurements in air were taken from the same places where soil samples were taken. Average outdoor gamma dose rates in sample stations were determined as 67 nGy h(-1). The annual effective dose to the public was found to be 82 microSv.     

Fractionation of natural radionuclides in soils from the vicinity of a former uranium mine ?irovski vrh, Slovenia

As a result of former uranium mining and milling activities at ?irovski vrh, Slovenia, 0.6 million tons of uranium mill tailings (UMT) were deposited onto a nearby waste pile Boršt. Resulting enhanced levels of natural radionuclides in UMT could pose threat for the surrounding environment. Therefore, sequential extraction protocol was performed to assess mobility and bioavailability of ²³⁸U, ²³⁴U, ²³⁰Th and ²²⁶Ra in soils from the waste pile and its surrounding. The radionuclides associated with exchangeable, organic, carbonate, Fe/Mn oxides and residual fraction, respectively, were determined. Results showed that the highest activity concentrations for the studied radionuclides were on the bottom of the waste pile. In non-contaminated locations, about 80% of all radionuclides were in the residual fraction. Considering activity concentrations in the UMT, ²³⁸U and ²³⁴U are the most mobile. Mobility of ²²⁶Ra is suppressed by high sulphate concentrations and is similar to mobility of ²³⁰Th.     

Aerial measurements on uranium ore mining, milling and processing areas in Germany

The paper describes aerial measurements at several sites containing residues from uranium mines, waste rock dumps and tailings ponds of the Wismut company in Saxony and Thuringia. For the measurements, a computerized gamma-ray spectrometer equipped with a HPGe-detector and a NaI(Tl)-detector array with a volume of 121 was used. Radioactive anomalies from natural radionuclides have been detected and mapped. The activity concentrations of 226Ra, 228Th and 40K in areas with elevated radioactivity from natural radionuclides were determined from aerial measurements. Ground-based measurements--as far as available--confirmed these results. The mean 226Ra activity concentrations in the different waste rock dumps were found to be in the range 370 to 1600 Bq kg-1. The highest mean 226Ra activity concentrations were measured for the tailings ponds with values up to 1300 Bq kg-1. For 40K and 208Tl, activity concentrations of 860 and 40 Bq kg-1, respectively, were obtained as averages of all measurements. These values are commonly found in the environment. In general, there is reasonable agreement between the results measured with different detectors and measuring methods.     

Radiological maps for Trabzon, Turkey

The activity concentrations and absorbed gamma dose rates due to primordial radionuclides and ¹³⁷Cs have been ascertained in 222 soil samples in 18 counties of the Trabzon province of Turkey using a HPGe detector. The mean activity concentrations of ²³⁸U, ²³²Th, ⁴⁰K and ¹³⁷Cs in soil samples were 41, 35, 437 and 21 Bq kg⁻¹, respectively. Based on the measured concentrations of these radionuclides, the mean absorbed gamma dose in air was calculated as 59 nGy h⁻¹ and hence, the mean annual effective dose due to terrestrial gamma radiation was calculated as 72 μSv y⁻¹. In addition, outdoor in situ gamma dose rate (D) measurements were performed in the same 222 locations using a portable NaI detector and the annual effective dose was calculated to be 66 μSv y⁻¹ from these results. The results presented in this study are compared with other parts of Turkey. Radiological maps of the Trabzon province were composed using the results obtained from the study.     

Assessment of the radiological impacts of historical coal mining operations on the environment of Ny-Alesund, Svalbard

Mineral extraction activities, such as those conducted by oil, gas and coal industries, are widespread throughout the Arctic region. Waste products of these activities can result in significant contributions to the radioactive burden of the surrounding environment due to increased concentrations of naturally occurring radioactive materials (NORM) to levels that would not normally be found in the environment. Coal mining operations commenced in the early 1900s on Svalbard and have been conducted at a variety of locations on the archipelago since then. Coal contains radionuclides of the uranium and thorium series as well as 40K. Extraction and processing of coal can result in releases of these radionuclides to the broader environment with subsequent impact on the human and non-human inhabitants of the area. This paper presents the results of a study on environmental radioactivity resulting from historical coal mining operations conducted at Ny-Alesund, Spitsbergen, in the Svalbard archipelago. Activity concentrations of radionuclides found in materials associated with these operations are presented as well as the results of a spatial dosimetric survey conducted over an area affected by coal mining.     

Radioactive contamination in the marine environment adjacent to the outfall of the radioactive waste treatment plant at ATOMFLOT,northern Russia

RTP "ATOMFLOT" is a civilian nuclear icebreaker base located on the Kola Bay of northwest Russia. The objectives of this study were to determine the distributions of man-made radionuclides in the marine environment adjacent to the base, to explain the form of the distributions in sediments and to derive information concerning the fate of radionuclides discharged from ATOMFLOT. Mean activity concentrations (d.w.) for surface sediment, of 63 Bq kg(-1 137Cs, 5.8 Bq kg(-1) 90Sr and 0.45 Bq kg(-1 239,240)Pu were measured. Filtered seawater activity levels were in the range of 3--6.9 Bq m(-3) 137Cs, 2.0-11.2 Bq m(-3) 90Sr, and 16-40 m Bq m(-3), 239,240Pu. Short-lived radionuclides were present at sediment depths in excess of 10cm indicating a high degree of sediment mixing. Correlations of radionuclide activity concentrations with grain-size appear to be absent; instead, the presence of relatively contaminated sediment appears to be related to the existence of radioactive particles.     

Invariance of isotope ratios of lithogenic radionuclides: more evidence for their use as sediment source tracers

Activities of radionuclides in the 238U (230Th, 226Ra, 210Pb) and 232Th (232Th, 228Th, 228Ra) decay series were determined in sediments from an east Texas watershed and examined with isotope ratios and compared to particulate organic carbon (POC), % fines (<63 microm) and total concentrations of Al, Fe and Mn. The objective was to elucidate the presence or absence of relationships affecting the effectiveness of these radionuclides in modeling sediment transport. Strong positive correlations were observed between radionuclides and Mn (Th) and % fines (Ra and Th). Isotope ratios effectively reduce these influences, supporting the contention that isotope ratios offset extrinsic variability in terrestrial sediments. Strong associations of 210Pbxs (excess 210Pb) and 226Ra/230Th with POC agree with data from marine and terrestrial settings, indicating that the role of POC in isotope fractionation, transport and sequestration merits further investigation.     

Radiochemical analyses for environmental radiological studies at nuclear power stations

The analytical procedures used in a program of radiological monitoring studies at nuclear power stations are discussed. Samples of in-plant and effluent liquids, gases, and airborne particles were analyzed by radiochemical methods or by gamma-ray spectrometry. These procedures were modified for environmental media, including air, airborne particles, vegetation and food, milk, animal tissue, water, soil and sediment, generally by analyzing larger samples, enhancing the purification procedures, and increasing the detection sensitivity. Emphasis was placed on analyzing special samples for effluent radionuclides not routinely monitored, such as gaseous H-3, C-14, and Kr-85, and on measuring radionuclides at very low concentrations in media of possible dosimetric significance, such as radioiodine in milk. Measurements at these low levels permitted comparisons of source terms with environmental radioactivity in terms of calculational models.     

Concentration ratios for small mammals collected from the exposed sediments of a 137Cs contaminated reservoir

(137)Cs concentration ratios were computed for small mammals collected from the dried sediments of a partially drained, contaminated reservoir. Soil (137)Cs activity concentrations were heterogeneous on small and large spatial scales and had a geometric mean of 253 (range 23-2110) Bq/kg dry weight. Mean (137)Cs activity concentrations in composite cotton rat Sigmodon hispidus and cotton mouse Peromyscus gossypinus samples averaged 2480 (range 556-6670) and 471 (range 96-1000) Bq/kg whole body dry weight, respectively. About 50% of the variance in cotton rat tissue (137)Cs activity was explained by variation in soil (137)Cs activity. Soil-to-animal dry weight concentration ratios averaged 6.0 for cotton rats and 1.2 for cotton mice and were generally similar to (137)Cs concentration ratios for herbivorous, homeothermic animals from other contaminated ecosystems. In the RESRAD-BIOTA dose model, the default wet-weight concentration ratio for (137)Cs in terrestrial animals is 110 resulting in an estimate of internal and external radiation doses to terrestrial biota that is 44 times more than the dose calculated with the actual measured wet-weight concentration ratio for cotton rats (1.6). These results show that site-specific concentration ratios can significantly affect the estimation of dose.