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.     

Results of the European Commission MARINA II study: part I--general information and effects of discharges by the nuclear industry

From the collated data relevant to discharges by the nuclear industry, it results that the input of beta activity (excluding Chernobyl fallout and tritium) into the OSPAR region decreased by a factor of 4 from 1986 to 1991, reaching by this date the same level as in the early 1950s. Over the same period the discharges of the alpha activity into the OSPAR region also decreased by a factor 3, the same trend has been seen also for tritium. Since 1986 the effective dose to members of the critical group in the vicinity of Sellafield and Cap de La Hague was consistently below the ICRP and EU limit of 1 mSv per year to members of the general public. The overall radiological impact from nuclear industry on the population of the European Union from the OSPAR area has decreased from 280 manSv y(-1) in 1978 to 14 manSv y(-1) in 2000.     

Exposure of biota in the cooling pond of Ignalina NPP: hydrophytes

The radiological assessment of non-human biota is now accepted by a number of international bodies. In this connection the scientific basis to assess and evaluate biota internal and external radiation exposure is required. This paper presents the comparison of freshwater biota (hydrophyte species) exposure due to discharged anthropogenic radionuclides with that due to natural background radiation. The radionuclides from Ignalina Nuclear Power Plant (Lithuania) are discharged into cooling pond - Druksiai Lake. Submerged hydrophytes were selected as biota exposure indicators because they represent the largest biomass in this lake and have comparatively high radionuclide activity concentrations. The detailed methodology evaluation of the submerged hydrophyte dose rate is presented. The ionizing radiation exposure dose rates to submerged hydrophyte roots and above sediment parts due to the major radionuclides ((54)Mn, (60)Co, (137)Cs, (90)Sr) discharged into the INPP cooling pond - Druksiai Lake were 0.044 microGyh(-1) and 0.004 microGyh(-1), respectively. The internal exposure dose rate due to natural background alpha-emitters ((210)Po,(238)U, (226)Ra) was estimated to be 1.24 microGyh(-1), as compared with that of anthropogenic alpha-emitter (240)Pu - 0.04 microGyh(-1), whereas the external exposure was 0.069 microGyh(-1). The presented data deeper the knowledge about the concentration of radionuclides and submerged hydrophytes' exposure dose rates in European freshwater ecosystems.     

A regulatory perspective on the radiological impact of NORM industries: the case of the Spanish phosphate industry

Radioactive and chemical risks coexist in NORM industries although they are usually addressed separately by regulations. The European Union (EU) has developed extensive legislation concerning both matters, which has been diversely reflected in national policies. We consider the case of the Spanish phosphate industry and analyse to which extent regulatory mandates have reduced the historical and ongoing radiological impact on the environment of phosphate facilities. Although no specific radiological constraints on effluent monitoring and release or on waste disposal have yet been imposed on NORM industries in Spain, other environmental regulations have achieved a substantial reduction on the phosphate industry impact. Nevertheless, a more efficient control could be established by eliminating the current conceptual and practical separation of chemical and radioactive risks in NORM industries. We highlight research needs to accomplish so and propose shorter-term measures that require active cooperation among the regulatory bodies involved.     

Radiological impact from atmospheric releases of 238U and 226Ra from phosphate rock processing plants

Phosphate rocks are used extensively, mainly as a source of phosphorus for fertilizers and secondarily for phosphoric acid and other speciality chemicals. Phosphates are typically enriched in uranium and are thus one of the sources of technologically enhanced natural radiation (TENR) which increases exposure to man from natural radionuclides. Emissions from phosphate rock processing plants in gaseous and particulate form contain radionuclides, such as 238U and 226Ra, which are discharged into the environment causing radiation exposures to the population. About 10 MBq each of 238U and 226Ra are discharged into the environment each year from SICNG, a phosphate rock processing plant in Thessaloniki area, Northern Greece. The collective dose commitment to lung tissue resulting from atmospheric releases was estimated to be approximately 2 x 10(-9) person Gy t-1 for 238U and approximately 0.1 x 10(-9) person Gy t-1 for 226Ra, i.e. about 2 times higher than that estimated in the UNSCEAR reports issued in 1982, 1988, and 1993.     

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).     

Distribution of natural radionuclides in the production and use of phosphate fertilizers in Brazil

The Brazilian phosphate fertilizer is obtained by wet reaction of igneous phosphate rock with concentrated sulphuric acid, giving as final product, phosphoric acid and dehydrated calcium sulphate (phosphogypsum) as by-products. Phosphoric acid is the starting material for triple superphosphate (TSP), single superphosphate (SSP), monoammonium phosphate (MAP) and diammonium phosphate (DAP). The phosphate rock used as raw material presents in its composition radionuclides of the U and Th natural series. Taking this into account, the main aim of this paper is to evaluate the fluxes of natural radionuclides and radioactive disequilibria involved in the Brazilian industrial process of phosphoric acid production; to determine the content of radioactivity in several commercial fertilizers produced by this industry; to estimate their radiological impact in crop soils and the long term exposure due to their application. Radiological characterization of phosphate rock, phosphogypsum and phosphate fertilizers was performed by alpha and gamma spectrometry. The fertilizer samples, which are derived directly from phosphoric acid, MAP and DAP, presented in their composition low activity concentrations for 226Ra, 228Ra and 210Pb. As for U and Th, the concentrations found in MAP and DAP are more significant, up to 822 and 850Bqkg(-1), respectively. SSP and TSP, which are obtained by mixing phosphoric acid with different amounts of phosphate rock, presented higher concentrations of radionuclides, up to 1158Bqkg(-1) for (238)U, 1167Bqkg(-1) for (234)U, 1169Bqkg(-1) for 230Th, 879Bqkg(-1) for 226Ra, 1255Bqkg(-1) for 210Pb, 521Bqkg(-1) for 232Th, 246Bqkg(-1) for 228Ra and 302Bqkg(-1) for 228Th. Long term exposure due to successive fertilizer applications was evaluated. Internal doses due to the application of phosphate fertilizer for 10, 50 and 100 years were below 1mSvy(-1), showing that the radiological impact of such practice is negligible.     

Partitioning of radionuclides and trace elements in phosphogypsum and its source materials based on sequential extraction methods

Phosphogypsum is a waste produced by the phosphate fertilizer industry. Although phosphogypsum is mainly calcium sulphate dihydrate, it contains elevated levels of impurities, which originate from the source phosphate rock used in the phosphoric acid production. Among these impurities, radionuclides from 238U and 232Th decay series are of most concern due to their radiotoxicity. Other elements, such as rare earth elements (REE) and Ba are also enriched in the phosphogypsum. The bioavailability of radionuclides (226Ra, 210Pb and 232Th), rare earth elements and Ba to the surrounding aquatic system was evaluated by the application of sequential leaching of the phosphogypsum samples from the Brazilian phosphoric acid producers. The sequential extraction results show that most of the radium and lead are located in the "iron oxide" (non-CaSO4) fraction, and that only 13-18% of these radionuclides are distributed in the most labile fraction. Th, REE and Ba were found predominantly in the residual phase, which corresponds to a small fraction of the phosphate rock or monazite that did not react and to insoluble compounds such as sulphates, phosphates and silicates. It can be concluded that although all these elements are enriched in the phosphogypsum samples they are not associated with CaSO4 itself and therefore do not represent a threat to the surrounding aquatic environment.     

Natural radioactivity in phosphates, phosphogypsum and natural waters in Morocco

The contents of natural radionuclides (uranium, actinium and thorium series) were measured in sedimentary phosphate rock samples using high-resolution gamma spectrometry. Data obtained for uranium content (ppm) were compared with the results obtained by a method based on the measurements using solid-state nuclear track detectors (SSNTD) in the same samples. The potential leaching of radionuclides from sedimentary phosphate rock during the industrial production of the phosphoric acid was studied. The process of leaching of the radioisotopes from phosphogypsum was discussed. A method for the direct alpha counting of 226Ra thin source, elaborated by the deposition of Ra from aqueous solutions on manganese oxides film deposited on polyvinyl support, have been developed and applied for the determination of 226Ra in natural water samples. The results show that only the water sample from the mine area reveals the presence of 226Ra at a level of about 0.2 Bq l-1.     

Journal of Environmental Radioactivity special issue: international topical conference on Po and radioactive Pb isotopes

An international conference on polonium (Po) and radioactive isotopes was held in Seville Spain, 26-28 October 2009 at the Centro Nacional de Aceleradores. It was attended by 138 participants from 38 different countries. The sessions covered all aspects on Po and lead (Pb) such as radiochemistry, terrestrial and marine radioecology, kinetics, sedimentation rates, atmospheric tracers, NORM industries and dose assessment     

A box model for calculation of collective dose commitment from radioactive waterborne releases to the baltic sea

To meet the new regulations of maximum yearly releases from Swedish nuclear power plants issued by the Swedish National Radiation Protection Institute, and to make realistic calculations of collective dose commitment derived from radionuclides discharged to the Baltic Sea, a box model AQUAPATH-BALTIC has been developed. The model calculates radionuclide concentrations in 25 boxes for discharges into given compartments and takes into consideration the dispersion rates of the water masses, the sediment-water interaction and radioactive decay. The calculated concentrations in water and sediment at steady state are then used to evaluate individual and collective intakes of activity and external exposures. The radiation doses to the global population following discharges to the Baltic Sea are also calculated.     

Evaluation of 210Pb and 210Po in cigarette tobacco produced in Brazil

Cigarette smoking is one of the pathways that might contribute significantly to the increase in the radiation dose reaching man, due to the relatively large concentrations of 210Pb and 210Po found in tobacco leaves. In the present study, the concentrations of these two radionuclides were determined in eight of the most frequently sold cigarette brands produced in Brazil. 210Pb was determined by counting the beta activity of 210Bi with a gas flow proportional detector after radiochemical separation and precipitation of PbCrO4. 210Po was determined by alpha spectrometry using a surface barrier detector after radiochemical separation and spontaneous deposition of Po on a copper disk. The results showed concentrations ranging from 11.9 to 30.2 mBq per gram of dry tobacco for 210Pb and from 10.9 to 27.4 mBq per gram of dry tobacco for 210Po. The collective committed effective dose resulting from the use of cigarettes produced in Brazil per year is estimated to be 1.5 x 10(4) man-Sv.     

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.     

Nuclide migration and the environmental radiochemistry of Florida phosphogypsum

Phosphogypsum, a waste by-product derived from the wet process production of phosphoric acid, represents one of the most serious problems facing the phosphate industry in Florida today. This by-product gypsum precipitates during the reaction of sulfuric acid with phosphate rock and is stored at a rate of about 40 million tons per year on several stacks in central and northern Florida. The main problem associated with this material concerns the relatively high levels of natural uranium-series radionuclides and other impurities which could have an impact on the environment and prevent its commercial use. We have studied the potential release of radionuclides from phosphogypsum by: (i) analysis of stack fluids, groundwaters, and soils associated with gypsum stacks; and (ii) geochemical modeling. Stack fluids were observed to be very high in dissolved uranium and 210Pb with only moderate concentrations of 226Ra. Underlying soils tend to be enriched in U and 210Pb indicating precipitation when acidic stack fluids enter a buffered environment. Modeling results showed significant increases in radionuclide complexes with sulfate and phosphate, resulting in relatively mobile uncharged or negatively charged solution species within the stacks with likely precipitation of multicomponent solids with increasing pH below the stack. Our evidence thus suggests that, while phosphogypsum stacks do contain significant quantities of dissolved radionuclides, removal mechanisms appear to prevent large-scale migration of radionuclides to the underlying aquifer.     

Choosing an alpha radiation weighting factor for doses to non-human biota

The risk to non-human biota from exposure to ionizing radiation is of current international interest. In calculating radiation doses to humans, it is common to multiply the absorbed dose by a factor to account for the relative biological effectiveness (RBE) of the radiation type. However, there is no international consensus on the appropriate value of such a factor for weighting doses to non-human biota. This paper summarizes our review of the literature on experimentally determined RBEs for internally deposited alpha-emitting radionuclides. The relevancy of each experimental result in selecting a radiation weighting factor for doses from alpha particles in biota was judged on the basis of criteria established a priori. We recommend a nominal alpha radiation weighting factor of 5 for population-relevant deterministic and stochastic endpoints, but to reflect the limitations in the experimental data, uncertainty ranges of 1-10 and 1-20 were selected for population-relevant deterministic and stochastic endpoints, respectively.     

Transfer of radiocarbon liquid releases from the AREVA La Hague spent fuel reprocessing plant in the English Channel

The recent risk assessment by the North-Cotentin Radioecology Group (, 1999) outlined that (14)C has become one of the major sources of the low dose to man through seafood consumption. It was recommended that more data should be collected about (14)C in the local marine environment. The present study aims to respond to this recommendation. The estimation of (14)C activity in marine species is based on concentration factor values. The values reported here ranged from 1x10(3) to 5x10(3)Bqkg(-1)ww/BqL(-1). A comparison was made between the observed and predicted values. The accuracy of (14)C activity calculations was estimated between underestimation by a factor of 2 and over-estimation by 50% (95% confidence interval). However, the use of the concentration factor parameter is based on the biological and seawater compartments being in steady state. This assumption may not be met at short distances from the point of release of discharges, where rapid changes in seawater concentration may be smoothed out in living organisms due to transfer kinetics. The data processing technique, previously published by Fiévet and Plet (2003. Estimating biological half-lives of radionuclides in marine compartments from environmental time-series measurements. Journal of Environmental Radioactivity 65, 91-107), was used to deal with (14)C transfer kinetics, and carbon half-lives between seawater and a few biological compartments were thus estimated.     

MEAD (part II)-Predictions of radioactivity concentrations in the Irish Sea

The predictions from MEAD, a model that simulates the transport of radionuclides in the marine environment, are presented for the Irish Sea. MEAD predictions for (137)Cs and Pu(alpha) are presented following discharges from BNFL Sellafield and the predictions compared to measured data from near the discharge location and further a field in the Irish Sea. The model performs well in most circumstances given the uncertainties involved in both modelling and data collection although some inconsistencies in the predictions are found. MEAD is also compared to other models of radionuclide transport in the Irish Sea.     

Radioactive contamination in the Arctic--sources, dose assessment and potential risks

Arctic residents, whose diets comprise a large proportion of traditional terrestrial and freshwater foodstuffs, have received the highest radiation exposures to artificial radionuclides in the Arctic. Doses to members of both the average population and selected indigenous population groups in the Arctic depend on the rates of consumption of locally-derived terrestrial and freshwater foodstuffs, including reindeer/caribou meat, freshwater fish, goat cheese, berries, mushrooms and lamb. The vulnerability of arctic populations, especially indigenous peoples, to radiocaesium deposition is much greater than for temperate populations due to the importance of terrestrial, semi-natural exposure pathways where there is high radiocaesium transfer and a long ecological half-life for this radionuclide. In contrast, arctic residents with diets largely comprising marine foodstuffs have received comparatively low radiation exposures because of the lower levels of contamination of marine organisms. Using arctic-specific information, the predicted collective dose is five times higher than that estimated by UNSCEAR for temperate areas. The greatest threats to human health and the environment posed by human and industrial activities in the Arctic are associated with the potential for accidents in the civilian and military nuclear sectors. Of most concern are the consequences of potential accidents in nuclear power plant reactors, during the handling and storage of nuclear weapons, in the decommissioning of nuclear submarines and in the disposal of spent nuclear fuel from vessels. It is important to foster a close association between risk assessment and practical programmes for the purposes of improving monitoring, formulating response strategies and implementing action plans.     

Distribution of some natural gamma-emitting radionuclides in the soils of the coastal areas of Nigeria

Studies on the radiation level and the radionuclide distribution of some naturally occurring radioactive materials (NORM) in the soils of the coastal areas of Southern Nigeria were undertaken. The purpose of this study is to provide baseline data for the effective monitoring of unforeseeable radioactive fallout in these areas where a lot of oil exploration activities are going on. The radioactivity concentrations of these naturally occurring radionuclides (specifically (40)K, (238)U and (232)Th) in the soil samples were analyzed using a high-resolution, low-background, hyper-pure coaxial gamma-ray detector (EG&G ORTEC HPGe) coupled to an amplifier and multi-channel analyzer. The activity of (40)K ranges between 111.9 and 444.7 kBq kg(-1) with a median value of 283.28 kBq kg(-1); the activity of (226)Ra (a daughter of (238)U) varies from 23.24 to 43.66 kBq kg(-1) with a median value of 34.54 kBq kg(-1); and that of (232)Th ranges from 6.45 to 12.79 kBq kg(-1) with a median value of 9.17 kBq kg(-1). The mean absorbed dose rate in air due to these NORM is found to be (33.655+/-3.409) nGy h(-1). The correlation analyses showed a positive relationship between the three radionuclides in all the five coastal states.     

Environmental characterization and radio-ecological impacts of non-nuclear industries on the Red Sea coast

The Red Sea is a deep semi-enclosed and narrow basin connected to the Indian Ocean by a narrow sill in the south and to the Suez Canal in the north. Oil industries in the Gulf of Suez, phosphate ore mining activities in Safaga-Quseir region and intensified navigation activities are non-nuclear pollution sources that could have serious radiological impacts on the marine environment and the coastal ecosystems of the Red Sea. It is essential to establish the radiological base-line data, which does not exist yet, and to investigate the present radio-ecological impact of the non-nuclear industries to preserve and protect the coastal environment of the Red Sea. Some natural and man-made radionuclides have been measured in shore sediment samples collected from the Egyptian coast of the Red Sea. The specific activities of 226Ra and 210Pb (238U) series, 232Th series, 40K and 137Cs (Bq/kg dry weight) were measured using gamma ray spectrometers based on hyper-pure germanium detectors. The specific activities of 210Po (210Pb) and uranium isotopes (238U, 235U and 234U) (Bq/kg dry weight) were measured using alpha spectrometers based on surface barrier (PIPS) detectors after radiochemical separation. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of 228Ra/226Ra, 210Pb/226Ra, 226Ra/238U and 234U/238U were calculated for evaluation of the geo-chemical behaviour of these radionuclides. The average specific activity of 226Ra (238U) series, 232Th series, 40K and 210Pb were 24.7, 31.4, 427.5 and 25.6 Bq/kg, respectively. The concentration of 137Cs in the sediment samples was less than the lower limit of detection. The Red Sea coast is an arid region with very low rainfall and the sediment is mainly composed of sand. The specific activity of 238U, 235U and 234U were 25.3, 2.9 and 25.0 Bq/kg. The average specific activity ratios of 226Ra/228Ra, 210Pb/226Ra and 234U/238U were 1.67, 1.22 and 1.0, respectively. The relationship between 226Ra/228Ra activity ratio and sample locations along the coastal shoreline indicates the increase of this ratio in the direction of the Shuqeir in the north and Safaga in the south where the oil exploration and phosphate mining activities are located. These activities may contribute a high flux of 226Ra. The concentration and distribution pattern of 226Ra in sediment can be used to trace the radiological impact of the non-nuclear industries on the Red Sea coast.