Occurrence of 222Rn, 226Ra, 228Ra and U in groundwater in Fujian Province, China

222Rn, 226Ra, 228Ra and U were determined in a total of 552 groundwater samples collected throughout Fujian Province of China. The geometric mean concentrations of 222Rn, 226Ra, 228Ra and total U in the groundwater were 147.8 kBq m-3, 12.7 Bq m-3, 30.2 Bq m-3 and 0.54 microgram kg-1, respectively. High groundwater 222Rn was explained by the predominantly granitic rock aquifers in Fujian. A lifetime risk of 1.7 x 10(-3) was estimated for the ingestion of groundwater 222Rn. High ratios of 228Ra to 226Ra contents (geometric mean of 2.4) and their disproportion suggest that 228Ra should also be measured in the assessment of population doses from drinking water in the regions of high rock or soil 232Th. No significant correlation between the 222Rn concentrations in groundwater and air was found.     

Natural radionuclides in bottled water in Austria

Concentration levels of 226Ra, 222Rn and 210Pb were analyzed in domestic bottled waters commercially available in Austria. Concentrations up to 0.23 Bq/l, with a geometric mean of 0.041 Bq/l were found for 226Ra. Concentrations for 222Rn ranged from <0.12-18 Bq/l, the geometric mean being 0.54 Bq/l. Lead-210 was analyzed in selected samples, the concentrations ranging from <2 to 34 mBq/l, with a geometric mean of 4.7 mBq/l. Ingestion doses resulting from consumption of these waters were calculated for the geometric mean and the maximum concentrations of the three radionuclides. The effective dose equivalents for different age groups of the population due to the intake of 226Ra range from 0.001 to 0.22 mSv/y and of 210Pb from 0.0003 to 0.05 mSv/y. Ingestion doses from 222Rn are low compared to those from 226Ra and 210Pb, ranging from 0.0001 to 0.011 mSv/y for adults and children, respectively. The doses are compared to the total ingestion dose from dietary intake of natural radionuclides on an annual basis.     

Characterization of the TE-NORM waste associated with oil and natural gas production in Abu Rudeis, Egypt

The present study was conducted to characterize the Technically Enhanced Naturally Occurring Radioactive Materials (TE-NORM) waste generated from oil and gas production. The waste was characterized by means of dry screening solid fractionation, X-ray analysis (XRF and XRD) and gamma-ray spectrometry. Sediment of the TE-NORM waste was fractionated into ten fractions with particle sizes varying from less than 100 microm to more than 3 mm. The results showed that the TE-NORM waste contains mainly radionuclides of the 238U, 235U and 232Th series. The mean activity concentrations of 226Ra (of U-series), 228Ra (of Th-series) and 40K in the waste samples before fractionation (i.e. 3 mm) were found to amount to 68.9, 24 and 1.3 Bq/g (dry weight), respectively. After dry fractionation, the activity concentrations were widely distributed and enriched in certain fractions. This represented a 1.48 and 1.82-fold enrichment of 226Ra and 228Ra, respectively, in fraction F8 (2.0-2.5 mm) over those in bulk TE-NORM waste samples. The activity ratios of 238U/226Ra, 210Pb/226Ra, 223Ra/226Ra and 228Ra/224Ra were calculated and evaluated. Activity of the most hazardous radionuclide 226Ra was found to be higher than the exemption levels established by IAEA [International Atomic Energy Agency, 1994. International Basic Safety Standards for the Protection against Ionizing Radiation and for the Safety of Radiation Sources. GOV/2715/94, Vienna]. The radium equivalent activity (Ra-eq), radon (222Rn) emanation coefficient (EC) and absorbed dose rate (Dgammar) were estimated and these are further discussed.     

Natural radionuclides in drinking water supplies of São Paulo State, Brazil and consequent population doses

The activity concentrations of 228Ra, 226Ra and 222Rn have been analysed in 452 drinking water supplies of S?o Paulo State. This study started in 1994 and covered 54% of the 574 existing counties. Concentrations up to 235 and 131 mBq l-1 were observed for 226Ra and 228Ra, respectively, whereas 222Rn concentrations reached 315 Bq l-1. Radiation doses up to 0.3, 0.6 and 3.2 mSv yr-1 were estimated for the critical organs, for the ingestion of 226Ra, 226Ra and 222Rn, respectively. The corresponding committed effective doses reached values of 6 x 10(-3), 2 x 10(-2) and 3 x 10(-1) mSv yr-1, for the same radionuclides. These results indicate that 222Rn makes the highest contribution to the total effective dose.     

Primordial radionuclides in Canadian background sites: secular equilibrium and isotopic differences

A literature review and field sampling were done to obtain information on primordial (natural-series) radionuclide concentrations in terrestrial environments in diverse locations across Canada. Of special interest was the degree of secular equilibrium among members of decay series. The analytes measured in soils and plants were (nat)U by neutron activation-delayed neutron counting, (228)Th, (230)Th, (232)Th, (226)Ra and (210)Po by alpha spectroscopy, (210)Pb by gas flow proportional counting, (228)Ra by beta counting and (137)Cs by gamma spectroscopy. In addition, ICP-MS was used to obtain concentrations of about 50 analytes including elemental U, Pb, and Th. Samples were from seven representative background sites with a total of 162 plant samples from 38 different species. These data were supplemented by a review that gathered a large portion of the similar data from published sources. The sites chosen were semi-natural, far from any nuclear industry, although several were specifically located in areas with slightly elevated natural U concentrations. As might be expected, there were many cases of non-detectable concentrations. However, certain trends were evident. The activity ratio (210)Po/(210)Pb was unity in soils and non-annual plant tissues such as lichens. It was about 0.6 in annual plant tissues. These results are consistent with the time required for ingrowth of (210)Po to reach secular equilibrium. There was evidence from several sources that (210)Pb in plants came predominantly from deposition of (210)Pb from air after the decay of airborne (222)Rn. This was expected. Somewhat unexpected was the observation that (228)Th seemed to be much more plant available than (232)Th, even though both are in the same decay series and should be chemically similar. The difference was attributed to the combined effects of ingrowth from (228)Ra in the plant and effects of alpha recoil in mobilizing (228)Th in the soil. In general, the results of this study will benefit risk assessment, both in providing background concentrations, but also some indication of where isotope activity ratios can and cannot be used to estimate concentrations.     

Present status of 222Rn in groundwater in Extremadura

Radon-222 was measured in groundwater sources of Extremadura (Spain), analyzing 350 samples from private and public springs, wells, and spas by liquid scintillation counting (LSC) and gamma spectrometry. The (222)Rn activity concentrations ranged from 0.24 to 1168BqL(-1). The statistical analysis showed a log-normal distribution with a mean of (111+/-7)BqL(-1) and a median of (36+/-3)BqL(-1). A hydrogeological study revealed correlations between the activity concentration and the aquifer material's characteristics. A map of (222)Rn in groundwater was elaborated and compared with the natural gamma radiation map for this region. About 35% of the samples showed (222)Rn activity concentrations above the Euratom recommended limit of 100BqL(-1). Three uranium series radionuclides ((238)U, (234)U, and (226)Ra) were also assayed by alpha-particle spectrometry, estimating the annual effective dose due to the presence of these natural radionuclides in drinking water.     

Natural radioactivity in the scale of water well pipes

The natural radioactivity of 226Ra and 228Ra in scale samples taken from pipes used in several local water wells was investigated. The results showed 226Ra activities to be varying from 1284 to 3613 Bq/kg whereas, the 228Ra concentrations did not show any significant variation, all being low, below 30 Bq/kg. The 222Rn exhalations from these scale samples were also measured and compared with the 226Ra contents. The average ratio of 222Rn/226Ra was 31%. Chemical analyses showed that the main constituent of the scale samples was iron. The radiation dose rates from the pipes and scale were up to 100nSv/h. Although not a major hazard this could present a long-term risk if the scale materials were handled indiscriminately.     

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.     

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.     

Reconnaissance of submarine groundwater discharge at Ubatuba coast,Brazil, using 222Rn as a natural tracer

Submarine groundwater discharge (SGD), which includes fresh groundwater and recycled seawater, has been recognized as a widespread phenomenon that can provide important chemical elements to the ocean. Several studies have demonstrated that SGD may approach or even exceed freshwater sources in supplying nutrients to coastal zones. This work reports preliminary results of a study carried out in a series of small embayments of Ubatuba, S?o Paulo State, Brazil, covering latitudes between 23 degrees 26'S and 23 degrees 46'S and longitudes between 45 degrees 02'W and 45 degrees 11'W. The main aims of this research were to set up an analytical method to assess 222Rn and 226Ra activities in seawater samples and to apply the excess 222Rn inventories obtained to estimate SGD. Measurements made during the summer of 2001 included 222Rn and 226Ra in seawater, 226Ra in sediment, seawater and sediment physical properties, nutrients and seepage rates. A continuous 222Rn monitor was also used to determine in situ collection of data to study short-term changes at one location. All methods indicated significant inflow of subsurface fluids at rates in excess of several cm per day.     

Natural radionuclides in Austrian mineral water and their sequential measurement by fast methods

Ten samples of Austrian mineral water were investigated with regard to the natural radionuclides (228)Ra, (226)Ra, (210)Pb, (210)Po, (238)U and (234)U. The radium isotopes as well as (210)Pb were measured by liquid scintillation counting (LSC) after separation on a membrane loaded with element-selective particles (Empore Radium Disks) and (210)Po was determined by alpha-spectroscopy after spontaneous deposition onto a copper planchette. Uranium was determined by ICP-MS as well as by alpha-spectroscopy after ion separation and microprecipitation with NdF(3). From the measured activity concentrations the committed effective doses for adults and babies were calculated and compared to the total indicative dose of 0.1 mSv/a given in the EC Drinking Water Directive as a maximum dose. The dominant portion of the committed effective dose was due to the radium isotopes; the dose from (228)Ra in most samples clearly exceeded the dose from (226)Ra.     

Radiological impacts of natural radioactivity in Abu-Tartor phosphate deposits, Egypt.

Phosphate and environmental samples were collected from Abu Tartor phosphate mine and the surrounding region. The activity concentration of 226Ra (238U) series, 232Th series and 40K were measured using a gamma-ray spectrometer. The activities of uranium isotopes (238U, 235U and 234U) and 210Pb were measured using an alpha spectrometer and a low-background proportional gas counting system, respectively, after radiochemical separation. The results are discussed and compared with the levels in phosphate rocks from different countries. It seems that the Abu Tartor phosphate deposit has the lowest radioactivity level of exploited phosphate of sedimentary origin. 226Ra/238U, 210Pb/226Ra, 234U/238U and 226Ra/228Ra activity ratios were calculated and are discussed. The radioactivity levels in the surrounding region and the calculated exposure dose (nGy/h) will be considered as a pre-operational baseline to estimate the possible radiological impacts due to mining, processing and future phosphate industrial activities. To minimize these impacts, the processing wastes should be recycled to the greatest possible extent.     

Daily ingestion of 232Th, 238U, 226Ra, 228Ra and 210Pb in vegetables by inhabitants of Rio de Janeiro City

The concentrations of the naturally occurring radionuclides 232Th, 238U, 210Pb, 226Ra and 238Ra were determined in the vegetables (leafy vegetables, fruit, root, bean and rice) and derived products (sugar, coffee, manioc flour, wheat flour, corn flour and pasta) consumed most by the adult inhabitants of Rio de Janeiro City. A total of 88 samples from 26 different vegetables and derived products were analyzed. The highest contribution to radionuclide intake arises from bean, wheat flour, manioc flour, carrot, rice, tomato and potato consumption. The estimated daily intakes due to the consumption of vegetables and derived products are 1.9 mBq of 232Th (0.47 microg), 2.0 mBq of 238U (0.17 microg), 19 mBq of 236Ra, 26 mBq of 210Pb and 47 mBq of 228Ra. The estimated annual effective dose due to the ingestion of vegetables and their derived products with the long-lived natural radionuclides is 14.5 microSv. Taking into account literature data for water and milk from Rio de Janeiro the dose value increases to 29 microSv, with vegetables and derived products responsible for 50% of the dose and water for 48%. 210Pb (62%) and 228Ra (24%) were found to be the main sources for internal irradiation.     

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.     

226Ra and 228Ra in scale and sludge samples and their correlation with the chemical composition

In order to contribute to a future waste management policy related to the presence of technologically enhanced natural occurring radioactive material (TENORM) in the Brazilian petroleum industry, the present work presents the chemical composition and the (226)Ra and (228)Ra content of sludge and scales generated during the offshore E and P petroleum activities in the Campos Basin, the primary offshore oil production region in Brazil. The (226)Ra and (228)Ra content on 36 sludge and scales samples were determined by gamma-spectrometry. Based on X-ray diffractometry results, a chemical analysis schema for these samples was developed. The results have shown that scales are 75% barium and strontium sulfates, with a mean (226)Ra and (228)Ra content of 106 kBq kg(-1) and 78 kBq kg(-1), respectively. On the other hand, sludge samples have a much more complex chemical composition than the scales. The (226)Ra and (228)Ra content in sludge also varies much more than the content observed in the scales samples and ranged from 0.36 to 367 kBq kg(-1) and 0.25 to 343 kBq kg(-1), respectively.     

(210)Pb content in natural gas pipeline residues ("black-powder") and its correlation with the chemical composition

The present work was carried out to assess the (210)Pb content in "black-powder" found in pigging operations on gas pipelines in Brazil, in particular, on the Campos Basin gas pipeline. Additionally, the chemical composition of such deposits was determined and an eventual correlation with (210)Pb concentration evaluated. Typical "black-powder" generated in the natural gas pipeline from Campos Basin oilfield contains mainly iron oxide ( approximately 81%) and residual organic matter ( approximately 9%). The (210)Pb content ranges from 4.9 to 0.04k Bqkg(-1) and seems to be inversely correlated with the distance to the platforms. On the other hand, (226)Ra concentration is higher on the pipeline branch between the platform and the onshore installations. (228)Ra was only observed in few samples, in particular, in the samples with the highest (226)Ra content.     

Radon emanation from NORM-contaminated pipe scale and soil at petroleum industry sites

Radon-222 emanation fractions were determined for barite scale deposits associated with petroleum production tubing and soil contaminated with naturally occurring radioactive material (NORM). Samples were analyzed for 226Ra concentration, the results of which were used to calculate the 222Rn emanation fraction for the sample. An important parameter determining the overall Rn activity flux from a solid medium, 222Rn emanation fraction represents the fraction of 222Rn produced that enters the interconnected pore space within a medium contaminated with 226Ra before the 222Rn undergoes radioactive decay. The primary objective of the study was to determine whether 222Rn emanation fractions from pipe scale and soil from petroleum production sites are similar to those of uranium mill tailings. Pipe scale samples were collected at four sites representing a wide geographical area, and consisted primarily of barite scale where Ra atoms have replaced a fraction of the Ba within the crystal lattice of the scale. Soil samples were collected at five sites, from areas exhibiting elevated surface gamma exposure rates indicating the presence of NORM. For comparison, 226Ra concentrations and 222Rn emanation fraction were also determined for uranium mill tailings samples provided from a site in Utah. Although 2226Ra concentrations from pipe scale samples were similar to those found in uranium mill tailings, 222Rn emanation fractions from scale were generally lower. Emanation fractions from each data set were statistically different from those of mill tailings (p < or = 0.01). The differences are probably due to physical differences between the two media and to the method by which the Ra is deposited in the material. Radon emanation from soils was extremely variable owing not only to differences in physical and chemical soil properties, but also to the means by which NORM has entered the soil. Although additional emanation measurements from other sites are needed, the data collected at these sites indicate that regulations intended to protect human health from 222Rn inhalation should consider the type and properties of the medium in which the NORM is contained, rather than relying strictly on concentrations of the parent 226Ra.     

Natural radionuclides in Brazilian mineral water and consequent doses to the population

Based on production data published by the Brazilian Mineral Water Producers Association, bottled mineral waters were bought at the market, covering, at least, 50% of the annual production of each Brazilian geographical region. 228Ra, 226Ra and 210Pb were analyzed and the weighted mean values obtained for Brazilian mineral waters were 0.097, 0.027 and 0.066 Bq l-1 respectively. Individual effective dose rate estimates due to ingestion of mineral water in Brazil were of the order of 10-100 microSv yr-1, depending on the geographical region. Based on the available data, it was also possible to evaluate the per caput effective dose rate and the highest value obtained was 4.3 microSv yr-1 for the northern region.     

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.     

Significant radioactive contamination of soil around a coal-fired thermal power plant

Soil samples were collected around a coal-fired power plant from 81 different locations. Brown coal, unusually rich in uranium, is burnt in this plant that lies inside the confines of a small industrial town and has been operational since 1943. Activity concentrations of the radionuclides 238U, 226Ra, 232Th, 137Cs and 40K were determined in the samples. Considerably elevated concentrations of 238U and 226Ra have been found in most samples collected within the inhabited area. Concentrations of 235U and 226Ra in soil decreased regularly with increasing depth at many locations, which can be explained by fly-ash fallout. Concentrations of 235U and 226Ra in the top (0-5 cm depth) layer of soil in public areas inside the town are 4.7 times higher, on average, than those in the uncontaminated deeper layers, which means there is about 108 Bq kg(-1) surplus activity concentration above the geological background. A high emanation rate of 222Rn from the contaminated soil layers and significant disequilibrium between 238U and 226Ra activities in some kinds of samples have been found.