Radionuclide speciation and its relevance in environmental impact assessments

To assess the long-term environmental impact of radioactive contamination of ecosystems, information on source terms including radionuclide speciation, mobility and biological uptake is needed. A major fraction of refractory radionuclides released from nuclear sources such as nuclear weapons tests and reactor accidents is present as radioactive particles, whilst radionuclides are also present as colloids or low molecular mass species in effluents from nuclear installations. Low molecular mass species are more mobile (lower apparent K(d)) and bioavailable (higher apparent BCF) than colloids and particles. Soils and sediments act as sinks for particles and colloids. Due to particle weathering, associated radionuclides can be remobilised over time. Thus, information on particle characteristics such as composition, particle size, crystalline structures and oxidation states influencing weathering rates and subsequent mobilisation is essential. The present article summarises current knowledge on radioactive particles released from different sources, and the relevance of radionuclide speciation for mobility and biological uptake.     

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.     

Radioactivity in environmental samples: Calibration standards measurement methods,quality assurance,and data analysis

The numerous environmental radioactivity measurements made by and for the U.S. Environmental Protection Agency (U.S. EPA) include measurements on samples of water, urine, food, milk, and air filters. Calibration standards are listed which are available in the form of water solutions and soils for a wide range of radionuclides. Method validation procedures for U.S. EPA approval include protocol development and single-laboratory and multiple-laboratory evaluation for precision and accuracy. Interlaboratory comparison studies are conducted for both cross-check and performance evaluation samples and involve 295 federal, state, and local laboratories. For water samples, 80%–90% of the participating laboratories are within the control limits for most of the radionuclides measured; however, some problem areas exist, especially for radium-228 and strontium-89 and -90. For milk and food samples, more than 90% of the laboratories are within control limits for cobalt-60 and cesium-137 but some problems exist for the measurement of strontium-90, iodine-131, and potassium-40. For tritium, 91% of the laboratories are within the control limit for water samples and 87% are within the control limits for the urine samples. The laboratory performance for air filter samples shows some problems for gross beta, strontium-90 and cesium-137 measurements.     

Particle-size distribution of fission products in airborne dust collected at Tsukuba from April to June 1986

The radioactivity released by the reactor accident at Chernobyl was detected in surface air at Tsukuba, Japan. Gamma-spectrometry of airborne dust collected using aerodynamic separation showed higher concentrations of radionuclides in fine particles. The particle-size distribution of radionuclides changed with time.     

Speciation of radionuclides - analytical challenges within environmental impact and risk assessments

The mobility, biological uptake and accumulation of radionuclides are essentially dependent on the physico-chemical form of the nuclides. As a major fraction of refractory radionuclides released during historical nuclear events is associated with particles, a key analytical challenge within environmental impact and risk assessments is to characterise radioactive particles with respect to properties influencing particle weathering, remobilisation and the subsequent ecosystem transfer of associated radionuclides. Preanalysis techniques are needed to fractionate, identify and localize individual particles in contaminated samples. To obtain information on particle characteristics such as particle size distributions, structures, elemental and radionuclide particle composition as well as oxidation state of matrix elements, solid-state speciation techniques are needed. Electron microscopy as well as X-ray microscopic techniques utilising synchrotron X-ray radiation have proved most useful in providing such information. The present paper summarises the present status on advanced techniques and presents historical sources that have contributed to radioactive particle contamination.     

The influence of hot particle contamination on Sr and Cs transfers to milk and on time-integrated ingestion doses

Most models for transfers of radionuclides through the food chain typically assume that the radioactivity is initially deposited in chemically available forms. It is known, however, that releases of radionuclides in the form of hot particles may significantly influence their environmental transfers and uptake to the food chain. This study presents models for time changes in ⁹⁰Sr and ¹³⁷Cs in milk which incorporate hot particle contamination using observed rates of hot particle dissolution following the Chernobyl accident. A general equation is presented for the influence of hot particles on overall ingestion doses. As expected from previous work, fallout of hot particles significantly influences time changes in radionuclide activity concentrations in foodstuffs. It is also shown that incorporation of radionuclides in hot particles influences time-integrated ingestion doses. For a situation in which a large proportion (90–100%) of fallout is in slowly dissolving hot particles, time-integrated ingestion doses from ⁹⁰Sr and ¹³⁷Cs are reduced by a factor of approximately two compared to the case where all radioactivity is deposited in bioavailable forms. However, the influence of rapidly dissolving hot particles on time-integrated ingestion doses is relatively minor. Remaining significant uncertainties in dose estimates are discussed.     

Photon attenuation, natural radioactivity content and radon exhalation rate of building materials

High concentrations of natural radionuclides in building materials can result in high dose rates indoors, from both internal and external exposure. In dose calculations, the main radionuclides of interest are 226Ra, 232Th and 40K. Usually much attention is paid to 226Ra due to 222Rn exhalation and the subsequent internal exposure. Other radionuclides of the uranium series such as 238U and 210Pb, emitting low energy photons are not usually determined and an assumption of radioactive equilibrium is made. The above assumption is seldom checked mainly because of the difficulties in the gamma-spectroscopic analysis of low energy photons. For the determination of radionuclides emitting low-energy photons, in samples like building materials where intense self-absorption of the photons exists, a method for self-absorption correction has been developed. The method needs as input the linear attenuation coefficient mu for the material under analysis. This paper presents: 1. Correlations in the form mu = f(rho,E) developed for the estimation of the linear attenuation coefficient mu (cm(-1)), as a function of the material packing density p (g cm(-3)) and the photon energy E (keV), for building materials as well as other materials of environmental importance. 2. Gamma-spectroscopic analysis techniques used for the determination of 238U, 226Ra, 210Pb, 232Th and 40K in environmental samples, together with the results obtained from the analysis of building materials used in Greece, and industrial by-products used for the production of building materials. Among the techniques used, one is based on the direct determination of 226Ra and 235U from the analysis of the multiplet photopeak at approximarely186 keV. 3. Results from radon exhalation measurements of building materials such as cement and fly-ash and building structures conducted in the radon chambers in our Laboratory. Based on the above results, dosimetric calculations are also reported.     

Critical analysis of radiochemical methodologies for the assessment of sediment pollution and dynamics in the lagoon of Venice (Italy)

Aquatic sediments are the ultimate sink of wastes dispersed in freshwater and soil. They are therefore a useful tool for investigating polluted ecosystems. Lagoon environments are very difficult to study due to their unstable morphology. Under these circumstances, even an excellent environmental investigation of a restricted lagoon area would still be inadequate to appreciate the characteristics of the entire system. The Venice lagoon is a very complex ecosystem whose morphology is complicated further by extensive anthropic intervention. A good environmental representation of the area was obtained with a preliminary radiochemical survey of airborne radionuclides, a unique tool in evaluating the homogeneity of the entire sedimentary system. It must be stressed, however, that the significance of the data depends substantially on the use of qualified procedures. Based on this, a detailed study was carried out on selected homogeneous areas, reconstructing the inventories and fluxes of pollutants in the sediments. In this work the radiochemical approach to the environmental study of the Venice lagoon is examined.     

Artificial radioactivity in Cumbria: Summary of an assessment by measurement and modelling

At the Harwell laboratory, the distributions of the artificial radionuclides discharged by British Nuclear Fuels at Sellafield have been measured within Cumbria, with particular emphasis on the transfer between environmental media. The results of the measurements have been incorporated into a model of the Cumbrian environment.The object of this work is to estimate the radiological impact upon man by exploring the pathways leading to external irradiation, to inhalation and to the ingestion of foodstuffs.Distributions have been established for caesium-137, plutonium isotopes and americium-241. Transfer from sea to land, of actinide radioactivity discharged to the sea, occures on a very small scale. The relative contributions to deposition and airborne radioactivity from sea-to-land transfer, fallout from nuclear weapons testing and atmospheric releases from Sellafield are compared. The dose resulting from sea-to-land transfer of actinides to a resident of Seascale peaked in 1973 at less than 1% of the ICRP annual limit for the general public and should fall steadily up to the year 2000.     

A survey of environmental radioactivity measurements in the United States

A survey of selected radiochemical laboratories in the United States was conducted to estimate the relative numbers and types of analyses performed nationwide for the measurement of environmental radio-activity and to identify the regulatory requirements which affect the selection of analytical procedures and media. Information was sought from each laboratory regarding its parent facility, whether the laboratory performs its own analyses or contracts them out, and the technical and regulatory requirements for which the laboratory performed analyses.Analyses of water, air-particulate, and soil and sediment samples contribute the greatest workload. Many fewer vegetation, milk, diet, gas, or bioassay samples are processed. The most common measurements, especially for water, are for gross-α and gross-β activity. More than 50 different specific-radionuclide analyses are being performed with varying degree of regularity by the 161 laboratories surveyed. γ-spectrometry is the most frequently used method for specific-radionuclide analyses; the use of Ge (Li) detectors for γ-spectrometric measurements now exceeds that of NaI (Tl) detectors. Other radionuclides for which specific analyses are frequently performed by a large percentage (25–75%) of the laboratories include ⁹⁰Sr, ¹³¹I, ²²⁶Ra, ^238,239Pu, ^234,235,238U, and tritium in water (HTO).     

Environmental radiation protection: philosophy, monitoring and standards

The Euratom Treaty confers important powers to the European Commission with regard to monitoring and assessment of levels of radioactivity in the environment and discharges with effluents (Articles 35-37 of the Euratom Treaty). Current developments in the area relate to harmonised reporting of environmental data and to harmonisation of effluent monitoring data. Both developments relate to the requirement under the new Basic Safety Standards (BSS) for a realistic assessment of population exposure. Guidance to this effect is being prepared by the Article 31 Group of Experts. In the context of Article 36 intercomparison exercises for radionuclides measurements in environmental samples are organised. New challenges for environmental monitoring result from the requirement under the BSS to regulate also industries processing NORM materials. Also the international move towards extending the scope of environmental radioactivity to the protection of biota opens new perspectives.     

The radiological impact from airborne routine discharges of a modern coal-fired power plant

In this paper the radiological impact from the airborne routine discharges of a modern coal-fired power plant at Langerlo (Belgium) is evaluated. Therefore, the natural radioactivity contents of the coal and the fly-ash discharged were measured. With a bi-Gaussian plume model the maximum annual values of the 226Ra concentration in the air (4.5 nBq/m3) and of the total deposition (1.5 mBq/m2) were calculated. The transfer of the radionuclides from air and soil to the biospheric media, exposing man, were modelled and the annual, individual, effective dose to the critical group, after an assumed life span of the power plant of 70 years, was evaluated at 0.05 microSv/y. This is several orders of magnitude lower than the annual doses for most power plants reported in the literature. The flue gas purification system, extended with a denitrification unit and a desulphurisation unit, was found to be the basis for this low impact.     

Studies on the distribution of 210Po and 210Pb in the ecosystem of Point Calimere Coast (Palk Strait), India

A systematic study on the natural radionuclides such as 210Po and 210Pb in the environmental matrices of Point Calimere ecosystem has been undertaken to establish a baseline data on the radiation profile of Point Calimere environment. The environmental samples such as water, sediment and biota (seaweeds, crustaceans, molluscs and fish) have been subjected to analyses. It has been observed that the concentration of 210Po and 210Pb in the water samples of Point Calimere to be 0.5 mBq/l and 1.3 mBq/l, respectively. The soft tissues of the organisms accumulated higher 210Po content while shells and bones contained more 210Pb. The bivalve molluscs Meretrix casta have been identified to accumulate higher concentration of 210Po suggesting that they could serve as bio-indicator of radionuclides like 210Po in the Point Calimere ecosystem. The concentration factor of 210Po for the biotic components ranged from approximately 10(3) to 10(6) while for 210Pb it ranged from approximately 10(3) to 10(5).     

Radioactive discharges from an alkaline pulp mill located in the south of Spain

Artificial and natural radionuclides present in environmental samples (Eucalyptus wood and bark) can be transferred in an alkaline pulp mill and concentrated in the recycling process. Some part of the radionuclides can be released into the environment associated with the discharges from such a factory. An alkaline pulp mill located in the South of Spain was extensively sampled during 1993 and different radionuclides analysed in the collected samples. Thus the concentrations and fluxes of natural (40K, 226Ra, 228Ra and 228Th) and artificial (137Cs and 90Sr) radionuclides associated with the samples collected along the pulp production process are presented. It is shown that radium and thorium radionuclides behave similarly to strontium and calcium and, consequently, concentrate within the Ca-cycle. Furthermore, 40K and 137Cs are concentrated during the Na-cycle. Finally, the results obtained by the authors are compared with the levels found in similar factories, though situated in the North of Europe, by other researchers.     

Aerial measurements of artificial radionuclides in Germany in case of a nuclear accident

Gamma-ray spectrometric systems carried by helicopters prove to be indispensable for the surveillance of environmental radioactivity. The aerial measurements are an important tool for rapid and large-scale nuclide specific determination of soil contamination after an accidental release of radionuclides from a nuclear facility. Furthermore this technique is also applied for the determination of anomalies of elevated radioactivity of natural radionuclides, the detection of lost radioactive sources and geological mapping. For the measurements the helicopters are equipped with a NaI(Tl)-detector array and a high purity germanium-semiconductor (HPGe) detector. Especially with the HPGe-detector it is possible to clearly identify individual radionuclides. To improve and to guarantee the quality of this method several exercises with different fields of interest have been carried out during the last years. Thereby the main focus is on the improvement of the instrumentation, data handling and data analysis. The results of the airborne radionuclide measurements from the Black Forest which was performed in co-operation with the Swiss National Emergency Operation Centre, are presented here. During this exercise the gamma dose rate, soil contamination due to 137Cs and the specific activities of natural radionuclides in soil were determined.     

NARAC: an emergency response resource for predicting the atmospheric dispersion and assessing the consequences of airborne radionuclides

The National Atmospheric Release Advisory Center (NARAC) serves as a national resource for the United States, providing tools and services to quickly predict the environmental contamination and health effects caused by airborne radionuclides, and to provide scientifically based guidance to emergency managers for the protection of human life. NARAC's scientists have developed a diverse tool kit of numerical modeling capabilities to respond to different types of release events, distance scales (local, regional, continental, and global), and response times.     

Validation of the ICRP model for caesium intake by lactating mothers with Italian data after the Chernobyl fallout

In the aftermath of the Chernobyl nuclear power plant accident, a research group of the Italian National Institute of Health (Istituto Superiore di Sanità) carried out two research programmes on maternal milk. One concerned the transfer of caesium radionuclides from the diet to breast milk. In the other, the activity concentrations of ¹³⁷Cs were also determined in urine and placenta. The first study estimated the mothers’ average ¹³⁷Cs dietary intake, in the second study the intake was evaluated individually for each subject. In 2004, the International Commission on Radiological Protection published modified systemic biokinetic models which also account for transfer to breast milk. The model for caesium radionuclides was implemented and tested by the authors with the experimental data described above. A good agreement was obtained between measured data and model simulations of ¹³⁷Cs activity concentration in human milk. The model, however, tends to systematically overestimate ¹³⁷Cs activity concentration in urine, in which case the agreement is to be considered satisfactory in terms of order of magnitude.     

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).     

Radionuclide transfer to animal products: revised recommended transfer coefficient values

A compilation has been undertaken of data which can be used to derive animal product transfer coefficients for radionuclides, including an extensive review of Russian language information. The resultant database has been used to provide recommended transfer coefficient values for a range of radionuclides to (i) cow, sheep and goat milk, (ii) meat (muscle) of cattle, sheep, goats, pigs and poultry and (iii) eggs. The values are used in a new IAEA handbook on transfer parameters which replaces that referred to as ‘TRS 364’. The paper outlines the approaches and procedures used to identify and collate data, and assumptions used. There are notable differences between the TRS 364 ‘expected’ values and the recommended values in the revised Handbook from the new database. Of the recommended values, three milk values are at least an order of magnitude higher than the TRS 364 values (Cr, Pu (cow) Pu (sheep)) and one milk value is lower (Ni (cow)). For meat, four values (Am, Cd, Sb (beef) I (pork)) are at least an order of magnitude higher than the TRS 364 values and eight values are at least an order of magnitude lower (Ru, Pu (beef), Ru, Sr, Zn (sheep), Ru, Sr (pork), Mn (poultry)). Many data gaps remain.     

Presence and behavior of organic pollutants in an aqueous environment surrounded by an industrialized area

Water and sediment samples in a bay surrounded by heavily industrialized areas were analyzed by a combined gas chromatography/mass spectrometry/computer system, and a number of aliphatic hydrocarbons, polycyclic aromatic hydrocarbons (PAH), and polar oxygenated compounds were found. Behavior of PAH in the bay and its surroundings was traced by gas chromatographic fingerprint by using a glass capillary column. Water and sediment, dust fall, and airborne particulate samples were used as environmental samples. It was emphatically suggested that the major origin of sedimentary PAH was airborne dust.