Radiological impact of coal-fired power generation

A radiological impact assessment was carried out at the 4000 MW Nanticoke Thermal Generating Station on the north shore of Lake Erie and at an ash disposal site in Metropolitan Toronto, both operated by Ontario Hydro. Analyses were performed on feed coal, fly ash and bottom ash and on samples of air filters, precipitation, water, soil and vegetation in the vicinity of the generating station. The measured radionuclide levels in the vicinity of the generating station showed no evidence of enhancement from station emissions. There were no indications that leaching of radionuclides or emanation of radon gas from ash disposal sites would be a problem. There was evidence, however, of higher radionuclide concentrations on the finer ash particles. Furthermore, the use of fly ash in building materials could lead to enhanced radiation levels. Atmospheric dispersion and radiation dose calculations were also carried out. Predicted concentrations in air were all less than 1% of background values. The committed dose equivalent from one year of operation was estimated to be 0·27 μSv at the site boundary and 0·11 μSv at 10 km east of the site.     

Escaping radioactivity from coal-fired power plants (CPPs) due to coal burning and the associated hazards: a review

Coal, like most materials found in nature, contains trace quantities of the naturally occurring primordial radionuclides, i.e. of ⁴⁰K and of ²³⁸U, ²³²Th and their decay products. Therefore, the combustion of coal results in the released into the environment of some natural radioactivity (1.48 TBq y⁻¹), the major part of which (99 %) escapes as very fine particles, while the rest in fly ash. The activity concentrations of natural radionuclides measured in coals originated from coal mines in Greece varied from 117 to 435 Bq kg⁻¹ for ²³⁸U, from 44 to 255 Bq kg⁻¹ for ²²⁶Ra, from 59 to 205 Bq kg⁻¹ for ²¹⁰Pb, from 9 to 41 Bq kg⁻¹ for ²²⁸Ra (²³²Th) and from 59 to 227 Bq kg⁻¹ for ⁴⁰K. Fly ash escapes from the stacks of coal-fired power plants in a percentage of 3-1% of the total fly ash, in the better case. The natural radionuclide concentrations measured in fly ash produced and retained or escaped from coal-fired power plants in Greece varied from 263 to 950 Bq kg⁻¹ for ²³⁸U, from 142 to 605 Bq kg⁻¹ for ²²⁶Ra, from 133 to 428 Bq kg⁻¹ for ²¹⁰Pb, from 27 to 68 Bq kg⁻¹ for ²²⁸Ra (²³²Th) and from 204 to 382 Bq kg⁻¹ for ⁴⁰K. About 5% of the total ash produced in the coal-fired power plants is used as substitute of cement in concrete for the construction of dwellings, and may affect indoor radiation doses from external irradiation and the inhalation of radon decay products (internal irradiation) is the most significant. The resulting normalized collective effective doses were 6 and 0.5 man-Sv (GW a)⁻¹ for typical old and modern coal-fired power plants, respectively.     

Gamma radioactivity in the Iberian Marine environment closest to the NEA dumping site

The distributions of caesium-137 and some naturally occurring gamma-emitters in a range of environmental samples, collected along the north-west Iberian coastline during April 1984, are presented. Samples, including surface waters, algae, sediments and fish, have been analyzed to establish accurate baselines for that region of the continental shelf closest to the NEA dumping site. Results indicate that caesium-137 levels were a factor of three lower than those typical of waters off the west coast of Ireland and are consistent with those expected from global fallout prior to the Chernobyl accident. The mean caesium-137 concentration in sea water at six well-separated stations near the coast was 3·85 ± 0·19 Bq m⁻³, whilst caesium-137 levels in widely consumed species of fish were in the range 1·1–6·2 Bq kg⁻¹ (dry wt). It is estimated that caesium-137, through one year's ingestion of fish and shellfish, generates a collective dose equivalent commitment to the adult Galician population of 0·78 man-Sv, which is approximately 3% of the total annula collective dose equivalent from non-medical sources of radiation.     

Radiation measurements and radioecological aspects of fallout from the cherbonyl reactor accident

Fallout from the Chernobyl reactor accident has been monitored for about one year in Thessaloniki in Northern Greece. Fifteen different short-lived, three relatively long- and one long-lived fission products were identified in air, precipitation, soil, grass and milk samples. The iodine-131 and cesium-137 concentrations in air reached 6·5 and 3 Bq m⁻³ respectively, on 6 May, 1986. The external exposure dose rate rose to five times the normal background level. It was estimated that the accumulated dose equivalent to the adult thyroid from inhaled iodine-131 averaged 96 μSv, while the body burden from inhaled radiocesium nuclides averaged 2 μSv, 1000 times lower than that corresponding to the estimated dose equivalent from ingestion of foodstuff, which averaged 2 mSv for the first year after the accident.     

Consequences of the Chernobyl reactor accident on the 137Cs internal dose to the Japanese population

The consequences of the Chernobyl reactor accident on the Japanese population are assessed here, for the one-year period from May 1986, in terms of the internal dose due to ¹³⁷Cs. The calculations are made via an approach which combines whole body counting with analysis of food intake data. First, the dose from ¹³⁷Cs is assessed, for a group of healthy adult males, on the basis of their observed body burdens of ¹³⁷Cs determined by whole body counting. The annual individual dose estimate thus obtained is 1·5 μSv, which is 6–15% and 3·7% respectively of the doses determined by whole body counting in UK and the Federal Republic of Germany. The temporal change in the average body burden is successfully explained here by a single-compartment model. Secondly, this latter model is used, along with the daily ¹³⁷Cs intake data for each district in Japan, to calculate the dose for the whole of Japan. Appropriate values were chosen for the relevant biological parameters for each age and sex group. The estimates of the population dose and the average individual dose thus obtained are 148 man Sv, for the population of 120 million, and 1·24 μSv, respectively. Although comparatively small, these values nonetheless also include the residual contribution from past nuclear weapon tests. The average annual individual dose of 1·24 μSv corresponds to 0·7% of the dose from natural ⁴⁰K in the body. Although whole body counting indicates that ¹³⁷Cs burdens were still increasing as of May 1987, it is concluded that, in terms of radiocaesium, the effect of the Chernobyl reactor accident on Japan was negligible.     

Migration of radium from the thorium ore deposit of Morro do Ferro,Poços de Caldas,Brazil

A large thorium ore deposit is located in Morro do Ferro, a hill in the Poços de Caldas Plateau, Minas Gerais, Brazil, which contains an estimated 30 000 t of Th and 100 t of U in a highly weathered matrix exposed to erosion and leaching. ²²⁸Ra and ²²⁶Ra were analyzed in surface waters collected at various points in the drainage basin and in groundwaters from wells drilled through and around the ore body. The concentrations in groundwater demonstrated that radium is markedly leached by rainwater percolating through the ore body. In its transit underground, radium is removed from groundwater by sorption on soil particles and this natural process greatly reduces the radium discharged to the environment. In dry weather, the concentration of dissolved ²²⁸Ra in the main stream draining the Morro do Ferro is 7·0 ± 1·1 mBq litre⁻¹ and in a control stream 1·6 ± 0·3 mBq litre⁻¹. The estimated ²²⁸Ra mobilization rate by solubilizations is of the order of 10⁻⁷ y⁻¹.     

Trace element and radionuclide mass balances at a coal-fired electric generating station

Coal, bottom ash, and fly ash from Milliken Station, a coal-fired 270 MW power plant, were analyzed for 20 elements (Ag, Al, As, Be, Cd, Co, Cr, Cu, Ga, Hg, Mn, Ni, Pb, Sb, Se, Sn, Te, Tl, V, and Zn) and the major natural radionuclides (²³⁸U series, ²³²Th series, and ⁴⁰K). Mass balance calculations showed that most of the Hg, and some of the Sb and Se, were unaccounted for by ash collection, suggesting their possible discharge into the atmosphere. Silver, As, Hg, Pb, Cd, and Zn were more concentrated in the fly ash than in the bottom ash while all of the other elements were equally distributed, by concentration, between the ash fractions. The radionuclides showed a 46% higher concentration in fly ash than in bottom ash, and ²¹⁰Pb was enriched in the fly ash relative to the other radionuclides by a factor of 2.4. Mass balance calculations indicated a balance within statistical error for the radionuclides, except for ²¹⁰Pb.     

Scavenging of 234Th in the Eastern Irish Sea

Measurements of the disequilibria of ²³⁴Th/²³⁸U in seawater and in suspended particulate and seabed sediment in the eastern Irish Sea reveal that the residence time of dissolved ²³⁴Th (0·5–7·7 days) is controlled by the concentration of particles in suspension (0·4–6·9 mg litre⁻¹, which reflects the rate of sediment resuspension (0·5–5·9 kg m⁻²y⁻¹). The residence time of ²³⁴Th with respect to removal to the seabed is longer (7–50 d) and is less dependent on variations in the suspended load. Anthropogenic sources of ²³⁸U contribute up to 8–15% of the water column production of ²³⁴Th. Enhanced scavenging occurs near the coast and there appears to be a net horizontal flux of ²³⁴Th within this region.     

Transfer of 241Am and 237Pu from euphausiid moults to a carbonate-rich marine sediment

Concentrations of ²⁴¹Am and ²³⁷Pu adsorbed onto moulted exoskeletons from the euphausiid Megancytiphanes norvegica decreased exponentially with 50% retention times of 3–7 d when moults were incubated in filtered seawater with small amounts of a carbonate-rich sediment. Over 95% of sediment weight was present as < 43 μm silt particles and 91 ± 4% of radioactivity lost from moults was recovered in this size fraction. Adsorption of both actinides (atoms μm⁻²) was greatest in the medium-fine sand fraction which had the highest carbonate content. These particles constituted <0·4% of total sediment dry weight but their reactivity (atoms μm⁻² surface: atoms μm⁻³ in solution) was 10³–10⁴ times higher than similar quotients for <43 μm particles. The enrichment shows that non-homogeneous distributions may arise between particle types when actinides such as ²⁴¹Am and ²³⁷Pu sorbed to surfaces of organic particles are transferred to sediments.     

Radon transport through a cool-season grass

²²²Rn released by mature tall fescue (Festuca arundinacea Schreb.) growing on uranium mill wastes in a controlled environment was a direct function of leaf area and essentially unrelated to the quantity of water transpired by the plants. The quantity of ²²²Rn released by the grass blades at maturity was approximately 0·01 Bq m⁻² s⁻¹ (0·3 pCi m⁻² s⁻¹). We suggest that the radioactive gas is transported from the rooting medium to leaves by mass flow in liquid water, but from leaves to the atmosphere by a path generally independent of water, i.e., primarily through the leaf cuticle and epicuticular wax.     

Carbon-14 discharges from the nuclear fuel cycle: 2. Local effects

Environemtnal ¹⁴C levels around various types of nuclear installations within the UK have been monitored during recent years. Enhanced ¹⁴C levels have been detected around both the nuclear fuel reprocessing plant as Sellafield and the thermal nuclear power station complex at Hunterston. From these measurements, the radiological impact of the ¹⁴C discharges on the local population is assessed. It is conservatively estimated that the ¹⁴CO₂ emissions from Sellafield between 1952 and 1985 could have delivered an 8·4 man Sv collective effective dose equivalent commitment to the population living within 40 km of the site. The maximum possible collective dose to the population within 15 km of Hunterston in 1984 was 15 × 10⁻³ man Sv. Conservative estimates of maximum annual effective dose equivalents to individuals around Sellafield and Hunterston are 0·2 mSv (in 1982) and 12 μSv (in 1984), respectively. These dose levels do not exceed the limits recommended by ICRP but the former value clearly indicates that, for the larger discharges at least, consideration and optimisation of ¹⁴C releases are fully justified. The same ¹⁴C measurements are also used to test the validity of two atmospheric dispersion models, the Gaussian plume and the so-called ‘hyperbolic’ models. The former is excellent in predicting downwind ¹⁴C levels around Hunterston but is unsatisfactory when applied to Sellafield, whereas the latter proves reliable at both sites. Further investigations suggest that the Gaussian plume model's poor performance at Sellafield can be explained by inaccurate input data.     

Fallout distribution in Padua and Northeast Italy after the chernobyl nuclear reactor accident

The radioactive cloud from the Chernobyl nuclear reactor accident arrived in northeast Italy on 30 April 1986. Ground-level air activities detected in Padua reached maximum values of 28·6, 19·2, 3·3, 1·7 and 7·5 Bq m⁻³ for ¹³¹I, ¹³²Te(¹³²I), ¹³⁷Cs and ¹⁰³Ru, respectively, on 1 May; about 10 days later, the activities had fallen to less than 1% of peak values. Considerations of cloud homogeneity are reported.The distribution of fallout radionuclides in Padua was evaluated on the basis of radioactivity detected on natural surfaces. The average committed dose equivalent to the thyroid for adult people in Padua through ¹³¹I inhalation was estimated at 0·37 mSv. Soil activity was monitored daily in samples collected in Padua during the first weeks of May 1986. Fallout deposition over northeast Italy was measured on 75 surface soil samples collected during June 1986 and long-lived radionuclide distribution maps were derived.     

Environmental radioactivity around tokai-works after the reactor accident at chernobyl

Following the reactor accident at Chernobyl, environmental samples of air, rain water and agricultural and marine products were collected and analyzed by gamma- and alpha-spectrometry. The highest concentrations of ¹³¹I in the environmental samples were as follows: 1·0×⁻¹ Bqm⁻³ (aerosol-associated in air); 3·0×10⁻¹ Bqm⁻³ (gaseous in air); 2·1×10² bq kg⁻¹ (plants); 1·4×10¹ Bq litre⁻¹ (milk). Other nuclides such as ⁹⁵Zr, ⁹⁵Nb, ¹⁰³Ru, ¹⁰⁶Ru, ¹²⁵Sb, ^129mTe, ¹³²I/¹³²Te, ¹³⁴Cs, ¹³⁷Cs, ¹⁴⁰Ba/¹⁴⁰La, ¹⁴¹Ce and ¹⁴⁴Ce were also observed in various environmental samples. ^110mAg was only detected in marine products such as cephalopoda and shellfish, ^239,240Pu and ²⁴¹Am originating from the accident were not identified.Based on the monitoring results at one dairy farm, we have derived an equation to model the transport of ¹³¹I from pasture grass to milk. This equation was then applied to the data from two other farms around Tokai-Works and the calculated ¹³¹I activities in milk were compared with those measured. The equation shows good predictive capabilities for quantification of the peak concentrations of ¹³¹I in milk but underestimates longer-term activities.     

UO22+-humate interactions in soft,acid, humate-rich waters

Few analytical techniques are sensitive enough to detect environmental concentrations of uranium in waters where humic acids are present. One objective of this study was to devise a technique for measuring humic-complexed and uncomplexed uranium at these concentrations. Three techniques were combined to determine the binding capacity and conditional stability constant of uranium with Aldrich^® humic acid. Free UO₂²⁺ was separated from bound by chelating resin; the CC bonds were destroyed by photo-oxidation and UO₂²⁺ was quantified by laser fluorometry. The binding capacity (BC) of 3·5 mg C liter⁻¹ Aldrich humic acid solution was estimated to be 1·14 × 10⁻⁶MUO₂²⁺ with an asymptotic standard error of 5·0 × 10⁻⁸MUO₂²⁺. UO₂²⁺ was bound to humic acid by a continuum of sites with different strengths. The frequency distribution of these sites was log-normal. A Gaussian-Scatchard model was used to estimate the overall conditional stability constant for uranium concentrations of 5·25 × 10⁻⁸Mto 2·1 × 10⁻⁷M in the presence of 3·5 mg liter⁻¹ humate (1·14 × 10⁻⁶M = φ). The estimates of the mean and standard deviation for the log of the stability constants were 6·5 and 0·8, respectively. When these mean and standard deviations were used to determine the mole-average number of binding sites at three points on the Gaussian distribution, the estimators of log-stability constants were found to be: K₁ = 5·2, K₂ = 6·5 andK₃ = 7·7 with mole fractions of the total number of binding sites associated with each region of 0·21, 0·55 and 0·21, respectively. The thermodynamic, geochemical simulation model GEOCHEM and the three-component Gaussian-Scatchard estimates allowed accurate prediction of the relative proportion of UO₂²⁺ bound to humates for a soft water pond across the entire range of metal-ligand ratios studied. Approximately 22% of the UO₂²⁺ was predicted to be associated with dissolved organic carbon.     

The transfer of 137Cs and 60Co from feed to pork

The transfer of ¹³⁷Cs and ⁶⁰Co from fodder to meat and other organs was studied in growing pigs. The influence of two different feeding methods (potato and grain) commonly used in Germany was investigated. The radionuclides were transferred into plants by root uptake and these were fed once a day, all at once, to young pigs until they reached maturity. In this manner, the radioactivity was administered to the pigs in a similar chemical form as would occur after radioactive contamination of soil. It is demonstrated that the two feeding practices have only a minor influence on transfer coefficients, which were determined to be ≤0·002 days/kg for ⁶⁰Co in meat and in the ranges 0·18–0·26 (potato-feeding) and 0·17–0·33 days/kg (grain-feeding), respectively, for ¹³⁷Cs in different components of the meat: the transfer coefficients for ¹³⁷Cs into different organs range from 0·06 to 0·24 days/kg after potato-feeding and from 0·12 to 0·29 after grain-feeding.     

Rare earth elements in fly ashes created during the coal burning process in certain coal-fired power plants operating in Poland - Upper Silesian Industrial Region

The subject of the study covered volatile ashes created during hard coal burning process in ash furnaces, in power plants operating in the Upper Silesian Industrial Region, Southern Poland. Coal-fired power plants are furnished with dust extracting devices, electro precipitators, with 99-99.6% combustion gas extracting efficiency. Activity concentrations ofTh-232, Ra-226, K-40, Ac-228, U-235 and U-238 were measured with gamma-ray spectrometer. Concentrations of selected rare soil elements (La, Ce, Nd, Sm, Y, Gd, Th, U) were analysed by means of instrumental neutron activation analysis (INAA). Mineral phases of individual ash particles were identified with the use of scanning electron microscope equipped with EDS attachment. Laser granulometric analyses were executed with the use of Analyssette analyser. The activity of the investigated fly-ash samples is several times higher than that of the bituminous coal samples; in the coal, the activities are: 226Ra - 85.4 Bq kg⁻¹, 40 K-689 Bq kg⁻¹, 232Th - 100.8 Bq kg⁻¹, 235U-13.5 Bq kg⁻¹, 238U-50 Bq kg⁻¹ and 228Ac - 82.4 Bq kg⁻¹.     

Uptake of 226Ra and 210Pb by food crops cultivated in a region of high natural radioactivity in Brazil

The Poços de Caldas Plateau is a deeply weathered alkaline igneous intrusion of about 35 km diameter, in which several radioactive anomalies exist. The first Brazilian uranium mine and mill are located in this region. A study is in progress to assess the edible vegetable uptake of the most abundant natural radionuclides in the local environment and this paper reports the results for ²²⁶Ra and ²¹⁰Pb. In farm soils, both nuclides have similar concentrations. The minimum values are comparable to those found in areas of normal radioactivity but the maximum concentrations are ten-fold higher. ‘Exchangeable’ radium in soils ranges from 2·3% to 34·5% of the total. No statistical correlation was found between the ‘exchangeable’ ²²⁶Ra and several physico-chemical soil parameters. In the vegetables analyzed, ²²⁶Ra concentrations are slightly higher than those of ²¹⁰Pb and the maximum values are also one order of magnitude greater than in normal regions. For both radionuclides, the average soil-to-plant concentration factors are of the order of 10⁻³ and 10⁻², when related to total and to ‘exchangeable’ contents in soils, respectively. For each vegetable, no statistical correlation was observed between the ²²⁶Ra or ²¹⁰Pb concentrations in the plant (fresh weight) and concentrations in the soil, either total or ‘exchangeable’. The ‘exchangeable’ Ca in soils does not seem to influence radium uptake by plants in a defined way.     

The distribution of plutonium,Americium and curium isotopes in pond and stream sediments of the Savannah river plant,South Carolina,USA

The concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am and ²⁴⁴Cm were determined in sediment samples from five streams and two ponds on the Savannah River Plant (SRP) and in four sediment samples from the Savannah River above and below the plant site. The following concentration ranges were determined: ²³⁸Pu, 0·07–386 fCi g⁻¹; ^239,240Pu, 0·37–1410 fCi g⁻¹; ²⁴¹Am, 0·1–4360 fCi g⁻¹; ²⁴⁴Cm, <0·01–392 fCi g⁻¹. Comparisons of the elemental and isotopic ratios of the sediments show that the majority of the sediments studied have been impacted upon by plant operations and that sediments outside the plant boundary in the Savannah River have only been influenced by aerial releases. Atom ratios of ²⁴⁰Pu/²³⁹Pu indicate that up to 86% of the Pu in these sediments is derived from plant operations. However, comparisons of the concentration data with values for other impacted sediments near nuclear facilities indicate that the levels are relatively small. Finally, <13% of the Pu, Am or Cm in pond sediments is associated with humic or fulvic acids, indicating that little of the material should be remobilized in oxic environments through organic complexation.     

Rapid remobilisation of plutonium from estuarine sediments

Plutonium remobilisation experiments, using contaminated Esk Estuary sediments and uncontaminated River Esk and North Sea waters, have successfully reproduced the observed non-conservative behaviour of dissolved Pu in the Esk Estuary, Cumbria, UK. Remobilisation is greatest at low salinites (<4%) and, under these conditions, Pu(III, IV) and Pu(V, VI) are released into solution in similar absolute amounts. The remobilisation process appears to be associated with a rapid (equilibrium achieved in 15 min) exchange reaction involving competition between Pu species, protons and major cations for the available surface sites. The experimental results show a systematic variation in distribution coefficients (i.e. K_d) for total Pu (7·2 × 10⁴−4·1 × 10⁶), Pu(III, IV) (1·0 × 10⁵−5·8 × 10⁶) and Pu(V, VI) (6·4 × 10³−5·5 × 10⁵).     

Radioecological consequences of radioactive discharges into the Techa River on the Southern Urals

The sources and levels of radioactive contamination of the Techa River are analyzed. Dose assessments are made for humams and biota. The highest radionuclide concentrations in the river water were observed in the period 1950–1951. In 1951, at a distance of 78 km from the site of radioactive discharges, the content of ⁹⁰Sr in the water was 2.7 × 10⁴ Bq l⁻¹ and that of ¹³⁷Cs was 7.5 × 10³ Bq l⁻¹. Subsequently, the radionuclide activity in the river water decreased considerably. In the period 1991–1994, the average annual content of ⁹⁰Sr in the water varied between 6 and 20 Bq l⁻¹. The average annual content of ¹³⁷Cs in the river water varied from 0.06 to 0.23 Bq l⁻¹, i.e. was lower than that of ⁹⁰Sr approximately by two orders of magnitude. The concentration of ^239,240Pu in the water varied between 0.004 and 0.019 Bq l⁻¹. The radioactive contamination of the Techa floodplain is highly nonuniform. With increasing distance from the river sources, the contamination density of the floodplain decreases, remaining, however, considerably higher than the background values.At present, the average annual dose rates in contaminated areas are (0.1–2) × 10⁻³ Sv year⁻¹, which is considerably lower than in the periods of ‘acute’ exposure (1950–1951). The doses to aquatic biota were much higher than those to humans.