Soil radium, soil gas radon and indoor radon empirical relationships to assist in post-closure impact assessment related to near-surface radioactive waste disposal

Least squares (LS), Theil’s (TS) and weighted total least squares (WTLS) regression analysis methods are used to develop empirical relationships between radium in the ground, radon in soil and radon in dwellings to assist in the post-closure assessment of indoor radon related to near-surface radioactive waste disposal at the Low Level Waste Repository in England. The data sets used are (i) estimated ²²⁶Ra in the <2 mm fraction of topsoils (eRa226) derived from equivalent uranium (eU) from airborne gamma spectrometry data, (ii) eRa226 derived from measurements of uranium in soil geochemical samples, (iii) soil gas radon and (iv) indoor radon data. For models comparing indoor radon and (i) eRa226 derived from airborne eU data and (ii) soil gas radon data, some of the geological groupings have significant slopes. For these groupings there is reasonable agreement in slope and intercept between the three regression analysis methods (LS, TS and WTLS). Relationships between radon in dwellings and radium in the ground or radon in soil differ depending on the characteristics of the underlying geological units, with more permeable units having steeper slopes and higher indoor radon concentrations for a given radium or soil gas radon concentration in the ground. The regression models comparing indoor radon with soil gas radon have intercepts close to 5 Bq m⁻³ whilst the intercepts for those comparing indoor radon with eRa226 from airborne eU vary from about 20 Bq m⁻³ for a moderately permeable geological unit to about 40 Bq m⁻³ for highly permeable limestone, implying unrealistically high contributions to indoor radon from sources other than the ground. An intercept value of 5 Bq m⁻³ is assumed as an appropriate mean value for the UK for sources of indoor radon other than radon from the ground, based on examination of UK data. Comparison with published data used to derive an average indoor radon: soil ²²⁶Ra ratio shows that whereas the published data are generally clustered with no obvious correlation, the data from this study have substantially different relationships depending largely on the permeability of the underlying geology. Models for the relatively impermeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with lower indoor radon: soil ²²⁶Ra ratios, whilst the models for the permeable geological units plot parallel to the average indoor radon: soil ²²⁶Ra model but with higher than average indoor radon: soil ²²⁶Ra ratios.     

Ra and Ra 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 ²²⁶Ra and ²²⁸Ra 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 ²²⁶Ra and ²²⁸Ra 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 ²²⁶Ra and ²²⁸Ra 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 ²²⁶Ra and ²²⁸Ra 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.     

Measurements of radiation level in petroleum products and wastes in Riyadh City Refinery

Recent concern has been devoted to the hazard arising from naturally occurring radioactive materials (NORM) in oil and gas facilities. Twenty-seven petroleum samples were collected from Riyadh Refinery. Fourteen samples were products and 13 were waste samples; three of them were scale samples and 10 were sludge samples. The specific radioactivities of (238)U, (232)Th, (226)Ra, (224)Ra, (40)K, and (235)U for all samples were determined using high-resolution gamma-ray spectrometry. The radium equivalent activity, radiation hazard indices and absorbed dose rate in air for all waste samples were estimated. The radon emanation coefficient of the waste samples was estimated. It ranged between 0.574 and 0.154. The age of two scale samples was determined and found to be 2.39 and 3.66 years. The chemical structure of the waste samples was investigated using X-ray florescence analysis (XRF) and Mg, Al, Si, S, Cl, Ca and Fe were found in all samples. From this study, it was noticed that the concentrations of the natural radionuclides in the petroleum wastes were higher than that of the petroleum products.     

External gamma-ray dose rate and radon concentration in indoor environments covered with Brazilian granites

Health hazard from natural radioactivity in Brazilian granites, covering the walls and floor in a typical dwelling room, was assessed by indirect methods to predict external gamma-ray dose rates and radon concentrations. The gamma-ray dose rate was estimated by a Monte Carlo simulation method and validated by in-situ measurements with a NaI spectrometer. Activity concentrations of ²³²Th, ²²⁶Ra, and ⁴⁰K in an extensive selection of Brazilian commercial granite samples measured by using gamma-ray spectrometry were found to be 4.5-450 Bq kg⁻¹, 4.9-160 Bq kg⁻¹ and 190-2029 Bq kg⁻¹, respectively. The maximum external gamma-ray dose rate from floor and walls covered with the Brazilian granites in the typical dwelling room (5.0 m × 4.0 m area, 2.8 m height) was found to be 120 nGy h⁻¹, which is comparable with the average worldwide exposure to external terrestrial radiation of 80 nGy h⁻¹ due to natural sources, proposed by United Nations Scientific Committee on the Effects of Atomic Radiation. Radon concentrations in the room were also estimated by a simple mass balance equation and exhalation rates calculated from the measured values of ²²⁶Ra concentrations and the material properties. The results showed that the radon concentration in the room ventilated adequately (0.5 h⁻¹) will be lower than 100 Bq m⁻³, value recommended as a reference level by the World Health Organization.     

Radium and uranium levels in vegetables grown using different farming management systems

Vegetables grown with phosphate fertilizer (conventional management), with bovine manure fertilization (organic management) and in a mineral nutrient solution (hydroponic) were analyzed and the concentrations of ²³⁸U, ²²⁶Ra and ²²⁸Ra in lettuce, carrots, and beans were compared. Lettuce from hydroponic farming system showed the lowest concentration of radionuclides 0.51 for ²²⁶Ra, 0.55 for ²²⁸Ra and 0.24 for ²³⁸U (Bq kg⁻¹ dry). Vegetables from organically and conventionally grown farming systems showed no differences in the concentration of radium and uranium. Relationships between uranium content in plants and exchangeable Ca and Mg in soil were found, whereas Ra in vegetables was inversely correlated to the cation exchange capacity of soil, leading to the assumption that by supplying carbonate and cations to soil, liming may cause an increase of U and a decrease of radium uptake by plants. The soil to plant transfer varied from 10⁻⁴ to 10⁻² for ²³⁸U and from 10⁻² to 10⁻¹ for ²²⁸Ra.     

Use of multitracers for the study of water mixing in the Paraíba do Sul River estuary

Multitracers were used to study water mixing in the Paraíba do Sul River estuary region in August 2007 (dry season) and March 2008 (rainy season) and to evaluate the reach of the river plume in the direction of the open ocean. Two sampling campaigns were carried out, each in a different season. Based on these results, it was possible to conclude that the multitracers used in this study (salinity, Si, Ba and U, as well as the radium isotopes ²²³Ra, ²²⁴Ra, ²²⁶Ra and ²²⁸Ra) presented satisfactory results toward defining the plume reach and determining the residence time and water-mixing processes in the estuary. A strong correlation was observed between tracers and the distance to the coast. During the low river water discharge period, the riverine water took about 10 days to reach open ocean waters (salinity ∼ 35). During the rainy period this value decreased to 6 days. Based on the radium results, it was possible to calculate diffusion coefficients (K_h) of 23 km² d⁻¹ and 38 km² d⁻¹ for ²²⁴Ra and ²²³Ra, respectively, during the dry season (winter). Values of 65 km² d⁻¹ and 68 km² d⁻¹ for ²²³Ra and ²²⁴Ra, respectively, were found for the rainy period (summer).     

Comparative study of natural radioactivity levels in soil samples from the Upper Siwaliks and Punjab,India using gamma-ray spectrometry

Natural radioactive materials under certain conditions can reach hazardous radiological levels. So, it becomes necessary to study the natural radioactivity levels in soil to assess the dose for the population in order to know the health risks and to have a baseline for future changes in the environmental radioactivity due to human activities. The natural radionuclide (²²⁶Ra, ²³²Th, and ⁴⁰K) contents in soil were determined for 26 locations around the Upper Siwaliks of Kala Amb, Nahan and Morni Hills, Northern India, using high-resolution gamma-ray spectrometric analysis. It was observed that the concentration of natural radionuclides viz., ²²⁶Ra, ²³²Th and ⁴⁰K, in the soil varies from 28.3 ± 0.5 to 81.0 ± 1.7 Bq kg⁻¹, 61.2 ± 1.3 to 140.3 ± 2.6 Bq kg⁻¹ and 363.4 ± 4.9 to 1002.2 ± 11.2 Bq kg⁻¹ respectively. The total absorbed dose rate calculated from activity concentration of ²²⁶Ra, ²³²Th and ⁴⁰K ranged from 71.1 to 162.0 nGy h⁻¹. The radium equivalent (R_eq) and the external hazard index (H_ex), which resulted from the natural radionuclides in soil, were also calculated and found to vary from 149.4 to 351.8 Bq kg⁻¹and from 0.40 to 0.95 respectively. These values in Upper Siwaliks area were compared with that from the adjoining areas of Punjab. The radium equivalent activities in all the soil samples were lower than the limit (370 Bq kg⁻¹) set in the Organization for Economic Cooperation and Development (OECD) report and the dose equivalent was within the safe limit of 1 mSv y⁻¹.     

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.     

Environmental fate of Ra in cation-exchange regeneration brine waste disposed to septic tanks, New Jersey Coastal Plain, USA: migration to the water table

Fate of radium (Ra) in liquid regeneration brine wastes from water softeners disposed to septic tanks in the New Jersey Coastal Plain was studied. Before treatment, combined Ra (²²⁶Ra plus ²²⁸Ra) concentrations (maximum, 1.54 Bq L⁻¹) exceeded the 0.185 Bq L⁻¹ Maximum Contaminant Level in 4 of 10 studied domestic-well waters (median pH, 4.90). At the water table downgradient from leachfields, combined Ra concentrations were low (commonly ≤0.019 Bq L⁻¹) when pH was >5.3, indicating sequestration; when pH was ≤5.3 (acidic), concentrations were elevated (maximum, 0.985 Bq L⁻¹ - greater than concentrations in corresponding discharged septic-tank effluents (maximum, 0.243 Bq L⁻¹)), indicating Ra mobilization from leachfield sediments. Confidence in quantification of Ra mass balance was reduced by study design limitations, including synoptic sampling of effluents and ground waters, and large uncertainties associated with analytical methods. The trend of Ra mobilization in acidic environments does match observations from regional water-quality assessments.     

Mapping radioactivity in groundwater to identify elevated exposure in remote and rural communities

A survey of radioactivity in groundwater (110 sites) was conducted as a precursor to providing a baseline of radiation exposure in rural and remote communities in Queensland, Australia, that may be impacted upon by exposure pathways associated with the supply, treatment, use and wastewater treatment of the resource. Radionuclides in groundwater, including ²³⁸U, ²²⁶Ra, ²²²Rn, ²²⁸Ra, ²²⁴Ra and ⁴⁰K were measured and found to contain activity concentration levels of up to 0.71 BqL⁻¹, 0.96 BqL⁻¹, 108 BqL⁻¹, 2.8 BqL⁻¹, 0.11 BqL⁻¹ and 0.19 BqL⁻¹ respectively. Activity concentration results were classified by aquifer lithology, showing correlation between increased radium isotope concentration and basic volcanic host rock. The groundwater survey and mapping results were further assessed using an investigation assessment tool to identify seven remote or rural communities that may require additional radiation dose assessment beyond that attributed to ingestion of potable water.     

Radium dial watches,a potentially hazardous legacy?

This study re-examines the risk to health from radium (²²⁶Ra) dial watches. Ambient dose equivalent rates have been measured for fifteen pocket watches giving results of up to 30 μSv h^− 1 at a distance of 2 cm taken with a series 1000 mini-rad from the front face (arithmetic mean ambient dose equivalent for pocket watches being 13.2 μSv h^− 1). A pocket compass gave rise to a similar ambient dose equivalent rate, of 20 μSv h^− 1, to the pocket watches, with its cover open. Eighteen wristwatches have also been assessed, but their dose rates are generally much lower (the arithmetic mean being 3.0 μSv h^− 1), although the highest ambient dose equivalent rate noted was 20 μSv h^− 1. A phantom experiment using a TLD suggested an effective dose equivalent of 2.2 mSv/y from a 1 μCi (37 kBq) radium dial worn for 16 h/day throughout the year (dose rate 0.375 μSv h^− 1). For this condition we estimated maximum skin dose for our pocket watches as 16 mSv per year, with effective doses of 5.1 mSv and 1.169 mSv when worn in vest and trouser pockets respectively. This assumes exposure from the back of the watch which is generally around 60–67% of that from the front. The maximum skin dose from a wristwatch was 14 mSv, with 4.2 mSv effective dose in vest pocket. Radium (²²⁶Ra) decays to the radioactive gas radon (²²²Rn), and atmospheric radon concentration measurements taken around a pocket watch in a small sealed glass sphere recorded 18,728 Bq m^− 3. All watches were placed in a room with a RAD7 real-time radon detector. Radon concentration average was 259 ± 9 Bq m^− 3 over 16 h, compared to background average over 24 h of 1.02 Bq m^− 3. Over 6 weeks highs of the order of 2000 Bq m^− 3 were routinely recorded when the heating/ventilation system in the room was operating at reduced rates, peaking at over 3000 Bq m^− 3 on several occasions. Estimates of the activity of ²²⁶Ra in the watches ranged from 0.063 to 1.063 μCi (2.31 to 39.31 kBq) for pocket watches and from 0.013 to 0.875 μCi (0.46 to 32.38 kBq) for wrist watches. The risk from old watches containing radium appears to have been largely forgotten today. This paper indicates a health risk, particular to collectors, but with knowledge and appropriate precautions the potential risks can be reduced.     

Natural radioactivity levels in topsoil from the Pearl River Delta Zone, Guangdong, China

Concentrations of the natural radionuclides ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K have been measured by γ-ray spectrometry in 796 topsoil samples from the Pearl River Delta Zone (PRDZ) of Guangdong, China. The mean concentrations for ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K were found to be 140 ± 37 Bq kg⁻¹, 134 ± 41 Bq kg⁻¹, 187 ± 80 Bq kg⁻¹ and 680 ± 203 Bq kg⁻¹ dry mass, respectively. These values were all higher than the mean values in soil for China and the world. Outdoor air-absorbed dose rates, calculated from activity concentrations of ²²⁶Ra, ²³²Th and ⁴⁰K, ranged from 86 to 237 nGy h⁻¹, with a mean value of 165 ± 46 nGy h⁻¹. The corresponding annual outdoor effective dose rate per person was estimated to be between 0.11 and 0.29 mSv y⁻¹, with a mean value of 0.20 ± 0.06 mSv y⁻¹, which was also higher than the world mean value of 0.07 mSv y⁻¹. The radium equivalent activity (Ra_eq) and the external hazard index (I_r) resulted from the natural radionuclides in soil, were also calculated and found to vary from 230 to 676 Bq kg⁻¹ and from 0.6 to 1.8, respectively. The Ra_eq and the I_r in all the investigated regions were up to 75% higher than the set limits of 370 Bq kg⁻¹ and 1.0, respectively.     

Relationship between deposition and attachment rates in Jacobi room model

It is shown in this work that parameters of the Jacobi model, which describes behavior of short-lived radon progeny, are not independent. The relationship between deposition rate of attached radon progeny and attachment rate of their unattached fraction was determined in this paper. It was found that deposition rate increases when the attachment rate is smaller; this effect is more pronounced for larger friction velocity. The deposition rate of attached radon progeny is presented here as a function of friction velocity, ventilation and attachment rate. Deposition rate of attached fraction was estimated in the range 0.012-0.46 h⁻¹, when attachment rate varies from 10 h⁻¹ to 100 h⁻¹.     

Radioactivity concentration in liquid and solid phases of scale and sludge generated in the petroleum industry

Scales and sludge generated during oil extraction and production can contain uranium, thorium, radium and other natural radionuclides, which can cause exposure of maintenance personnel. This work shows how the oil content can influence the results of measurements of radionuclide concentration in scale and sludge. Samples were taken from a PETROBRAS unit in Northeast Brazil. They were collected directly from the inner surface of water pipes or from barrels stored in the waste storage area of the E&P unit. The oil was separated from the solids with a Soxhlet extractor by using aguarras at 90+/-5 degrees C as solvent. Concentrations of 226Ra and 228Ra in the samples were determined before and after oil extraction by using an HPGe gamma spectrometric system. The results showed an increase in the radionuclide concentration in the solid (dry) phase, indicating that the above radionuclides concentrate mostly in the solid material.     

Studies on the Leaching of Radium and the emanation of radon from fertilizer process sludge

Radium-226 present in rock phosphate is carried to CaCO₃, the main process waste sludge of the fertilizer industry. Disposal of the sludge in the environment enhances the radiation background in the area. Two states of adherence of radium in the sludge have been identified, one loosely bound and the other chemically exchanged. The loosely bound fraction accounts for nearly 40% of the total activity, as demonstrated by leaching studies. Laboratory experiments show that activity leach-out by infiltration of water through the sludge is low. Lateral seepage is found to cause extensive areal contamination due to dispersal of suspended solids in the vicinity of the disposal area. The rate of emanation of radon from the sludge is found to be high, a factor of 10 over the normal background emanation rate. The radiation field in the waste disposal area also shows enhancement, with levels 4–6 times higher than natural background.     

Indoor air quality: Radon—Report on a WHO working group

The WHO Regional Office for Europe organized a working group in Dubrovnik, Yugoslavia, on 26–30 August 1985, which discussed radon as a pollutant affecting indoor air quality. Much of the natural background radiation to which the general public is exposed comes from the decay of ²²⁶Ra which produces radon gas and other products. Because radium is a trace element in most rock and soil, indoor concentrations of radon can come from a wide variety of substances, such as building materials and the soil under building foundations. Tap water taken from wells or underground springs may be an additional source. Radon daughter concentrations are considerably higher indoors than outdoors and are of the order of 2–5 Bq m⁻³ equilibrium equivalent radon (EER) concentration. It has been estimated that current exposure to radon gas could account for as much as 5–15% of all lung cancer deaths. It was recommended that, in general, buildings with concentrations of more than 100 Bq m⁻³ EER, as an annual average, should be considered for remedial action to lower such concentrations if simple measures are possible.     

Radiological monitoring: terrestrial natural radionuclides in Kinta District,Perak, Malaysia

Natural background gamma radiation and radioactivity concentrations were investigated from 2003 to 2005 in Kinta District, Perak, Malaysia. Sample locations were distant from any ‘amang’ processing plants. The external gamma dose rates ranged from 39 to 1039 nGy h⁻¹. The mean external gamma dose rate was 222 ± 191 nGy h⁻¹. Small areas of relatively enhanced activity were located having external gamma dose rates of up to 1039 ± 104 nGy h⁻¹. The activity concentrations of ²³⁸U, ²³²Th and ⁴⁰K were analyzed by using a high-resolution co-axial HPGe detector system. The activity concentration ranges were 12–426 Bq kg⁻¹ for ²³⁸U, 19–1377 Bq kg⁻¹ for ²³²Th and <19–2204 Bq kg⁻¹ for ⁴⁰ K. Based on the radioactivity levels determined, the gamma-absorbed dose rates in air at 1 m above the ground were calculated. The calculated dose rates and measured dose rates had a good correlation coefficient, R of 0.94. To evaluate the radiological hazard of the natural radioactivity, the radium equivalent activity, the gamma-absorbed dose rate and the mean population weighted dose rate were calculated. An isodose map for the Kinta District was also produced.     

A study of radium bioaccumulation in freshwater mussels, Velesunio angasi, in the Magela Creek catchment, Northern Territory, Australia

Freshwater mussels, Velesunio angasi, along Magela Creek in Australia’s Northern Territory were examined to study radionuclide activities in mussel flesh and to investigate whether the Ranger Uranium mine is contributing to the radium loads in mussels downstream of the mine. Radium loads in mussels of the same age were highest in Bowerbird Billabong, located 20 km upstream of the mine site. Variations in the ratio of [Ra]:[Ca] in filtered water at the sampling sites accounted for the variations found in mussel radium loads with natural increases in calcium (Ca) in surface waters in a downstream gradient along the Magela Creek catchment gradually reducing radium uptake in mussels. At Mudginberri Billabong, 12 km downstream of the mine, concentration factors for radium have not significantly changed over the past 25 years since the mine commenced operations and this, coupled with a gradual decrease of the ²²⁸Ra/²²⁶Ra activity ratios observed along the catchment, indicates that the ²²⁶Ra accumulated in mussels is of natural rather than mine origin. The ²²⁸Th/²²⁸Ra ratio has been used to model radium uptake and a radium biological half-life in mussels of approximately 13 years has been determined. The long biological half-life and the low Ca concentrations in the water account for the high radium concentration factor of 30,000-60,000 measured in mussels from the Magela Creek catchment.     

Dose estimation and radon action level problems due to nanosize radon progeny aerosols in underground manganese ore mine

One of the essential parameters influencing of the dose conversion factor is the ratio of unattached short-lived radon progeny. This may differ from the value identified for indoor conditions when considering special workplaces such as mines. Inevitably, application of the dose conversion factors used in surface workplaces considerably reduces the reliability of dose estimation in the case of mines.This paper surveyed the concentration of radon and its short-lived radon progeny and identified the unattached fraction of short-lived radon progeny. As well equilibrium factor during the month of August was calculated simultaneously at two extraction faces in a manganese ore mine.During working hours the average radon concentrations were 220 Bq m⁻³ and 530 Bq m⁻³ at Faces 1 and 2; the average short-lived progeny concentration was 90 Bq m⁻³ and 190 Bq m⁻³, the average equilibrium factors were 0.46 and 0.36, and the average unattached fractions were 0.21 and 0.17, respectively. The calculated dose conversion factor was between 9 and 27 mSv WLM⁻¹, but higher values could also be possible.     

Indoor radon levels in Greek schools

Radon and gamma dose rate measurements were performed in 512 schools in 8 of the 13 regions of Greece. The distribution of radon concentration was well described by a lognormal distribution. Most (86%) of the radon concentrations were between 60 and 250 Bq m⁻³ with a most probable value of 135 Bq m⁻³. The arithmetic and geometric means of the radon concentration are 149 Bq m⁻³ and 126 Bq m⁻³ respectively. The maximum measured radon gas concentration was 958 Bq m⁻³. As expected, no correlation between radon gas concentration and indoor gamma dose rate was observed. However, if only mean values for each region are considered, a linear correlation between radon gas concentration and gamma dose rate is apparent. Despite the fact that the results of radon concentration in schools cannot be applied directly for the estimation of radon concentration in homes, the results of the present survey indicate that it is desirable to perform an extended survey of indoor radon in homes for at least one region in Northern Greece.