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.     

Effect of moisture content on emanation at different grain size fractions - A pilot study on granitic esker sand sample

It is known that in soils and sediments moisture adsorbed on particle surfaces and in the pore system significantly affects the behaviour of recoiling radon (²²²Rn) atoms after decay of parent ²²⁶Ra, leading to increased ²²²Rn emanation. As a first step in an effort to characterize the ²²²Rn source term in mineralised sediments in the present study, complementing previous studies in the area, granitic esker sand samples were collected in order to test how moisture content affects ²²²Rn emanation at different grain size fractions. Emanation fractions measured for natural samples were compared with theoretical calculations. Six different grain size fractions were studied at 0%, 5% and 10% moisture contents relative to the mass of solids. In a further study necessary complementary information on the chemical and structural distribution of ²²⁶Ra was gained by selective leaching experiments. The results showed that ²²⁶Ra concentration increases from 50 Bq/kg at grain size 1-2 mm to 200 Bq/kg at grain size <0.063 mm. Respectively, the emanation factor increased from 0.12 to 0.30 at 5% moisture content. Both emanation factor and radium concentration increased significantly when grain size was below 0.125-0.250 mm. Above this fraction, the emanation fraction was approximately constant, 0.13 at 5% moisture content. In most of the grain size fractions, emanation reaches its maximum at 5% moisture content, being twice as high as in a dry sample. For the small particles (<0.063 mm) the ²²⁶Ra distribution is rather complex and depends on the mineral composition compared to larger particles wherein emanation from the internal pore system and the adjacent matrix is dominating over the contribution from external surface.     

Exhalation of (222)Rn from phosphogypsum piles located at the Southwest of Spain

Phosphogypsum (PG) is a waste product of the phosphoric acid production process and contains, generally, high activity concentrations of uranium series radionuclides. It is stored in piles formed over the last 40 years close to the town of Huelva (Southwest of Spain). The very broad expanse of the PG piles (about 1200 ha) produces a local, but unambiguous, radioactive impact to their surroundings. In 1992, the regional government of Andalusia restored an area of 400 ha by covering it with a 25-cm thick layer of natural soil and, currently, there is an additional zone of 400 ha in course of restoration (unrestored) and the same area of active PG stacks. Due to the high activity concentration of (226)Ra in active PG stacks (average 647 Bq kg(-1)), a significant exhalation of (222)Rn could be produced from the surface of the piles. Measurements have been made of (222)Rn exhalation from active PG stacks and from restored and unrestored zones. The (222)Rn exhalation from unrestored zones is half of that of the active PG stacks. Following restoration, the (222)Rn exhalation is approximately eight times lower than the active PG stacks. The activity concentrations of natural radionuclides ((226)Ra, (40)K, (232)Th) in the mentioned zones have been determined. This study was also conducted to determine the effect of (226)Ra activity concentration on the (222)Rn exhalation, and a good correlation was obtained between the (222)Rn exhalation and (226)Ra activity, porosity and density of soil.     

Natural radioactivity and radon exhalation in building materials used in Italian dwellings

Forty-two samples of building materials commonly used in Italian dwellings were surveyed for natural radioactivity. External (gamma), as defined and used by the European Commission, and internal (alpha) hazard indexes were calculated and radon specific exhalation rate and emanation fraction were measured. The accumulation method, by using the E-PERM electret ion chambers, was employed to determine specific exhalation rates of 222Rn. Several of the materials had hazard indexes that exceeded the European Commission limit values. However, it was evident that limit values for internal hazard indexes set based on Rn emanation should take into account the properties and use of the materials. For example, Rn emanation from basalt and glazed tiles was substantially lower than the Rn emanation from other materials with similar hazard indexes. Clearly there is need for improved guidelines and regulations in this area.     

Occupational dosimetric assessment (inhalation pathway) from the application of phosphogypsum in agriculture in South West Spain

Phosphogypsum (PG) has been traditionally applied as Ca-amendment in saline marsh soils in SW Spain, where available PG has 710 ± 40 Bq kg⁻¹ of ²²⁶Ra. This work assesses the potential radiological risk for farmers through ²²²Rn exhalation from PG-amended soils and by inhalation of PG-dust during its application. A three-year field experiment was conducted in a commercial farm involving two treatments: control and 25 t PG ha⁻¹ with three replicates (each 0.5 ha plots). The ²²²Rn exhalation rate was positively correlated with potential evapotranspiration, which explained 67% of the variability. Statistically significant differences between the control and PG treatments were not found for ²²²Rn exhalation rates, and mean values were within the lowest quartile of the typical range for ²²²Rn exhalation from soils. Airborne dust samples were collected during the application of PG and sugar-beet sludge amendments. The highest PG-attributable ²²⁶Ra concentration in the dust samples was 3.3 × 10² μBq m⁻³, implying negligible dose increment for exposed workers.     

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.     

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.     

Estimating the amount and distribution of radon flux density from the soil surface in China

Based on an idealized model, both the annual and the seasonal radon ((222)Rn) flux densities from the soil surface at 1099 sites in China were estimated by linking a database of soil (226)Ra content and a global ecosystems database. Digital maps of the (222)Rn flux density in China were constructed in a spatial resolution of 25 km x 25 km by interpolation among the estimated data. An area-weighted annual average (222)Rn flux density from the soil surface across China was estimated to be 29.7+/-9.4 mBq m(-2)s(-1). Both regional and seasonal variations in the (222)Rn flux densities are significant in China. Annual average flux densities in the southeastern and northwestern China are generally higher than those in other regions of China, because of high soil (226)Ra content in the southeastern area and high soil aridity in the northwestern one. The seasonal average flux density is generally higher in summer/spring than winter, since relatively higher soil temperature and lower soil water saturation in summer/spring than other seasons are common in China.     

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.     

Determination of specific activity of (226)Ra, (232)Th and (40)K for assessment of radiation hazards from Turkish pumice samples

The specific activity of (226)Ra, (232)Th and (40)K in 52 Turkish pumice samples collected from 11 geographical areas located in Central Anatolia, Eastern Anatolia, Mediterranean and Aegean regions was determined by gamma-ray spectrometry with a high-purity germanium (HPGe) detector. The specific activity of (226)Ra, (232)Th and (40)K ranged from 12.7+/-0.5 to 256.2+/-9.1Bqkg(-1) with a mean of 89.1+/-65.2Bqkg(-1), 12.3+/-1.0 to 237.9+/-12.2Bqkg(-1) with a mean of 87.0+/-61.4Bqkg(-1) and 300.1+/-5.5 to 1899.0+/-30.8Bqkg(-1) with a mean of 1211.9+/-419.8Bqkg(-1), respectively. Elemental concentrations were determined for U (from 1.0 to 20.7ppm with a mean of 7.2+/-5.3ppm), Th (from 3.0 to 58.6ppm with a mean of 21.4+/-15.1ppm) and K (from 1.0 to 6.1% with a mean of 3.9+/-1.3%). The radium equivalent activity (Ra(eq)), the activity index, the emanation coefficient, the (222)Rn mass exhalation rate, the indoor absorbed dose rate and the effective dose rate were estimated for the radiation hazard of the natural radioactivity in all samples. The calculated mean Ra(eq) value was 306.6+/-177.7Bqkg(-1) (54.6+/-5.5 to 737.6+/-49.0Bqkg(-1)) for all pumice samples. This value is lower than the recommended limit value of 370Bqkg(-1) for building raws and products. The emanation coefficient and the (222)Rn mass exhalation rate of all samples ranged from 29.4 to 42.9% with a mean of 36.2% and from 11.0 to 196.4muBqkg(-1)s(-1) with a mean of 73.5muBqkg(-1)s(-1), respectively. The mean indoor absorbed dose rate and the corresponding mean effective dose rate were 274.6+/-153.6nGyh(-1) (50.4-644.6nGyh(-1)) and 1.35+/-0.75mSvy(-1) (0.24-3.16mSvy(-1)), respectively. For all pumice samples the mean indoor absorbed dose rate is about three times higher than the population-weighted average of 84nGyh(-1), while the mean effective dose rate values except for PUM 05, PUM 06, PUM 10 and PUM 15 exceed the dose criterion of 1mSvy(-1).     

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.     

Assessment of the natural radioactivity and radiological hazards in Turkish cement and its raw materials

The natural radioactivity due to presence of (226)Ra, (232)Th and (40)K radionuclides in raw materials, intermediate products (clinker) and end products (22 different cement types) was measured using a gamma-ray spectrometry with HPGe detector. The specific radioactivity of (226)Ra, (232)Th and (40)K in the analyzed cement samples ranged from 12.5+/-0.3 to 162.5+/-1.7Bqkg(-1) with a mean of 40.5+/-26.7Bqkg(-1), 6.7+/-0.3 to 124.9+/-2.5Bqkg(-1) with a mean of 26.1+/-18.9Bqkg(-1) and 64.4+/-2.3 to 679.3+/-18.2Bqkg(-1) with a mean of 267.1+/-102.4Bqkg(-1), respectively. The radium equivalent activity (Ra(eq)), the gamma-index, the emanation coefficient, the (222)Rn mass exhalation rate and the indoor absorbed dose rate were estimated for the radiation hazard of the natural radioactivity in all samples. The calculated Ra(eq) values of cement samples (37.2+/-8.7-331.1+/-15.5Bqkg(-1) with a mean of 98.3+/-53.8) are lower than the limit of 370Bqkg(-1) set for building materials. The Ra(eq) values were compared with the corresponding values for cement of different countries. The mean indoor absorbed dose rate is slightly higher than the population-weighted average of 84nGyh(-1).     

Radon-222 exhalation from open ground on and around a uranium mine in the wet-dry tropics

Radon-222 exhalation from the ground surface depends upon a number of variables such as the 226Ra activity concentration and its distribution in soil grains; soil grain size; soil porosity, temperature and moisture; atmospheric pressure, rainfall and temperature. In this study, 222Rn exhalation flux density measurements within and around the Ranger uranium mine in northern Australia were performed to investigate the effect of these variables within a tropical region. Measurements were taken at the waste rock dumps, ore stockpiles, mine pits, and at sites where effluent water with elevated 226Ra concentration has been spray irrigated over land, as well as at sites outside the mine. The sites selected represented a variety of geomorphic regions ranging from uranium-bearing rocks to ambient soils. Generally, wet season rains reduced 222Rn exhalation but at a few sites the onset of rains caused a step rise in exhalation flux densities. The results show that parameters such as 226Ra activity concentration, soil grain size and soil porosity have a marked effect on 222Rn flux densities. For similar geomorphic sites, 226Ra activity concentration is a dominant factor, but soil grain size and porosity also influence 222Rn exhalation. Surfaces with vegetation showed higher exhalation flux densities than their barren counterparts, perhaps because the associated root structure increases soil porosity and moisture retention. Repeated measurements over one year at eight sites enabled an analysis of precipitation and soil moisture effects on 222Rn exhalation. Soil moisture depth profiles varied both between seasons and at different times during the wet season, indicating that factors such as duration, intensity and time between precipitation events can influence 222Rn flux densities considerably.     

Variations of the ambient dose equivalent rate in the ground level air

The ambient dose equivalent rate is caused by ionizing radiation of radionuclides in the atmosphere and on the ground surface as well as by cosmic radiation. Seasonal and diurnal variations of the ambient dose equivalent rate (ADER) in the ground level air are influenced by the concentration of 222Rn daughters. The 222Rn concentration in the ground level atmosphere, in turn, depends on the rate of the 222Rn exhalation from soil and turbulent air mixing. Its diurnal and seasonal variations depend on meteorological conditions. The aim of this study is to estimate the influence of variations of the rate of the 222Rn exhalation from soil and its concentrations in the ground level air on variations of ADER in the ground level air, as well as the dependence of these parameters on meteorological conditions. The 222Rn diffusion coefficient and its exhalation rate in undisturbed loamy soil have been determined. The 222Rn concentration in the soil air and its concentration in the ground level air correlate inversely (correlation coefficient is r = -0.62). The main factors determining the 222Rn exhalation from soil are: the soil temperature (r = 0.64), the difference in temperature of soil and air (r = 0.57), and the precipitation amount (r = 0.50). The intensity of gamma radiation in the ground level air is mostly related to the 222Rn concentration in the air (r = 0.62), while the effect of the exhalation rate from soil is relatively low (r = 0.36). It has been shown that ADER due to 222Rn progeny causes only 7-16% of the total ADER and influences its variation. The comparison of variations of ADER due to 222Rn progeny and the total ADER during several years shows that these parameters correlate positively.     

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.     

Radon, helium and CO2 measurements in soils overlying a former exploited oilfield, Pechelbronn district, Bas-Rhin, France

The Pechelbronn oilfield (Rhine Graben, France), where mining activity ended in the 1960s, has been used for waste disposal for twenty years. Since the wastes are varied, work is underway to identify the discharged materials and their derivatives, as well as to locate and quantify potential discharge sites. Two major goals were assigned to the present work. The first was to identify or refine the location of hidden structures that could facilitate gas emanation up to the surface, by studying soil gas concentrations (mainly ²²²Rn, CO₂, CH₄ and helium) and carbon isotope ratios in the CO₂ phase. The second was devoted to examining, from a health and safety viewpoint, if the use of the oilfield as a waste disposal site might have led to enhanced or modified gas emanation throughout the area.It appeared that CO₂ and ²²²Rn evolution in the whole area were similar, except near some of the faults and fractures that are known through surface mapping and underground observations. These ²²²Rn and CO₂ anomalies made it possible to highlight more emissive zones that are either related to main faults or to secondary fractures acting as migration pathways. In that sense, the CO₂ phase can be used to evaluate ²²²Rn activities distant from tectonic structures but can lead to erroneous evaluations near to gas migration pathways. Dumping of wastes, as well as oil residues, did not appear to have a strong influence on soil gaseous species and emanation. Similarly, enhanced gas migration due to underground galleries and exploitation wells has not been established. Carbon isotope ratios suggested a balance of biological phenomena, despite the high CO₂ contents reached. Other monitored gaseous species (N₂, Ar, H₂ and alkanes), when detected, always showed amounts close to those found subsurface and/or in atmospheric gases.     

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.     

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 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.     

A simple and rapid method for analyzing radon in coastal and ground waters using a radon-in-air monitor

We have developed a simple and portable technique for measuring moderately high levels of 222Rn (t1/2=3.8d) in natural waters such as coastal water, groundwater, and river water. The water sample is carefully collected in a glass bottle, and the sample bottle is connected to a radon-in-air monitor in a closed air-loop mode. By purging air through the sample, radon is emanated from the water until a chemical equilibration is obtained between the two phases. The radon in the air loop is determined using the radon-in-air monitor. Then, the radon in water is calculated by a radon-partitioning factor between water and air for a measured water temperature. This technique is especially convenient for determination of 222Rn in natural waters on field sites, since it eliminates the preparation of He gas, cold traps, and alpha-scintillation cells and counter, which are required for traditional radon emanation methods.