Liquid discharges from patients undergoing 131I treatments

This work discusses the production and management of liquid radioactive wastes as excretas from patients undergoing therapy procedures with (131)I radiopharmaceuticals in Spain. The activity in the sewage has been estimated with and without waste radioactive decay tanks. Two common therapy procedures have been considered, the thyroid cancer (4.14GBq administered per treatment), and the hyperthyroidism (414MBq administered per treatment). The calculations were based on measurements of external exposure around the 244 hyperthyroidism patients and 23 thyroid cancer patients. The estimated direct activity discharged to the sewage for two thyroid carcinomas and three hyperthyroidisms was 14.57GBq and 1.27GBq, respectively, per week; the annual doses received by the most exposed individual (sewage worker) were 164muSv and 13muSv, respectively. General equations to calculate the activity as a function of the number of patient treated each week were also obtained.     

Uranium isotopes in Tunisian bottled mineral waters

²³⁴U and ²³⁸U activity concentrations and their relative effective doses have been determined in 10 bottled mineral waters in Tunisia. Alpha spectrometry was used as technique to measure uranium isotopes. The obtained isotopic ratio ²³⁴U/²³⁸U varies between 1.1 and 3 which means that the two isotopes are not in radioactive equilibrium. Measured activity concentration varies between 3.2 and 40 mBq/l for ²³⁴U and between 1.5 and 26.3 mBq/l for ²³⁸U. Effective doses (assuming 2 litres per day of water consumption) coming from this two isotopes are found to vary between 0.16 and 2.02 μSv/a which is lower than the maximum recommended dose level by the WHO.     

Liquid discharges from the use of radionuclides in medicine (diagnosis)

The production and discharge of liquid radioactive wastes as excreta from patients undergoing Nuclear Medicine Diagnostic (NMD) in a hospital were studied. Instantaneous and accumulated activity, discharged from the hospital to the sewage system, has been estimated keeping in mind radionuclide decay. This study would enable estimation of the environmental impact due to NMD procedures. Annual accumulated activities of 2.2GBq ((131)I), 1.847GBq ((99m)Tc), 0.743GBq ((123)I), 0.337GBq ((67)Ga), 0.169GBq ((111)In) and 0.033GBq ((201)Tl) result from our model when applied to a European hospital. A comparison is made with calculations by other authors that do not consider the radionuclide decay and who overestimate by two orders of magnitude. Doses to critical people as sewage treatment workers are also significantly reduced. So, our results stress the importance of including the decay in the calculations.     

Plutonium isotopes in surface air of Prague in 1986–2006

Monitoring of ^239,240Pu in surface air of Prague started in 1986 in connection with the Chernobyl accident. Measurable activities of 10–28 μBq m⁻³ were found from 29 April 1986 to 5 May 1986. In the most of the monitoring periods of 1987–1996, activities of ^239,240Pu in air were not measurable. Positive values for ^239,240Pu and ²³⁸Pu in air could be obtained after installation of an aerosol sampler with higher flow-rate in 1997. Activity concentrations of ^239,240Pu and ²³⁸Pu in Prague air in the most of quarters of 1997–2006 were in the range 0.53–5.06 and <0.16–1.10 nBq m⁻³, respectively. Seasonal fluctuations can be found in content of ^239,240Pu in air. Activity ratios of ²³⁸Pu/^239,240Pu in air are higher than those in top soil, so it can be supposed that ²³⁸Pu is coming to air of Prague also from other sources than resuspension of fallout from atmospheric nuclear tests.     

Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA–UNESCO SGD project

Results of groundwater and seawater analyses for radioactive (³H, ²²²Rn, ²²³Ra, ²²⁴Ra, ²²⁶Ra, and ²²⁸Ra) and stable (D and ¹⁸O) isotopes are presented together with in situ spatial mapping and time series ²²²Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d⁻¹ to 360 cm d⁻¹; the unit represents cm³/cm²/day), as well as during a few hours (from 0 cm d⁻¹ to 110 cm d⁻¹), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous ²²²Rn measurements is 17 ± 10 cm d⁻¹. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7 × 10³ m³ d⁻¹ per km of the coast. The isotopic composition (δD and δ¹⁸O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of ²²²Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1–2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.     

Doses of external exposure in Jordan house due to gamma-emitting natural radionuclides in building materials

The use of building materials containing naturally occurring radionuclides as ⁴⁰K, ²³²Th, and ²³⁸U and their progeny results in external exposures of the residents of such buildings. In the present study, indoor dose rates for a typical Jordan concrete room are calculated using Monte Carlo method. Uniform chemical composition of the walls, floor and ceiling as well as uniform mass concentrations of the radionuclides in walls, floor and ceiling are assumed.Using activity concentrations of natural radionuclides typical for the Jordan houses and assuming them to be in secular equilibrium with their progeny, the maximum annual effective doses are estimated to be 0.16, 0.12 and 0.22 mSv a⁻¹ for ⁴⁰K, ²³²Th- and ²³⁸U-series, respectively. In a total, the maximum annual effective indoor dose due to external γ-radiation is 0.50 mSv a⁻¹. Additionally, organ dose coefficients are calculated for all organs considered in ICRP Publication 74. Breast, skin and eye lenses have the maximum equivalent dose rate values due to indoor exposures caused by the natural radionuclides, while equivalent dose rates for uterus, colon (LLI) and small intestine are found to be the smallest. More specifically, organ dose rates (nSv a⁻¹ per Bq kg⁻¹) vary from 0.044 to 0.060 for ⁴⁰K, from 0.44 to 0.60 for radionuclides from ²³⁸U-series and from 0.60 to 0.81 for radionuclides from ²³²Th-series.The obtained organ and effective dose conversion coefficients can be conveniently used in practical dose assessment tasks for the rooms of similar geometry and varying activity concentrations and local-specific occupancy factors.     

Population exposure to airborne thorium at the high natural radiation areas in India

High natural radiation areas in the coastal and peninsular India were studied for airborne thorium and resultant population exposure due to inhalation. Four locations covering three states viz., Ayiramthengu and Neendakara in Kerala, Kudiraimozhi in Tamil Nadu and Bhimilipatnam in Andhra Pradesh were investigated. External gamma radiation fields 1 m above the monazite ore bodies ranged from 200 to 3000 nGy h^-1. Soil samples showed ²³²Th specific activity varying from 0·1 to 1·5 Bq g^-1 with surface alpha activity in the range of 1·0–12·5 Bq cm^-2. Suspended particulates in the samples ranged from 60–140 μg m^-3 with ²³²Th showing a wider variation of <0·03–0·3 mBq m^-3. There was poor correlation between suspended particulates and long-lived alpha airborne activity . The resuspension factors for ²³²Th were in the range of 1·5×10^-8–7·9×10^-7 cm^-1. Higher resuspension was correlated with dry sand dunes. The upper limits for Committed Effective Dose (CED) due to inhalation of airborne ²³²Th at the respective high natural radiation areas were estimated to range from 50±30 to 300±130 μSv (5–30 mrem) per year per adult member of public assuming an activity median aerodynamic diameter of 1 μm for the airborne particulates.     

Behavior and analysis of Cesium adsorption on montmorillonite mineral

The adsorption of Cs by montmorillonite and the effects of experimental conditions on adsorption were investigated by using ¹³⁴Cs as a radioactive tracer. Additionally, the Cs-adsorbed and the modified montmorillonite were analyzed by X-ray Diffractometer System (XRD) and Scanning Electron Microscopy (SEM). The results showed that the adsorption of Cs by montmorillonite was efficient in the initial concentration (C₀) of 30 μg/L Cs nitrate solution with 20 g/L montmorillonite at room temperature. In this condition, more than 98% Cs⁺ ions could be adsorbed at pH 8. The adsorption equilibrium was achieved within 5 min and the relationship between the concentration of Cs⁺ in aqueous solutions and adsorption capacities of Cs⁺ can be described by the Langmuir adsorption isotherm. The adsorption rate would decrease when temperature increase from 0 °C to 50 °C or in presence of coexistent K⁺, Na⁺ and Ca²⁺, while modification by (NH₄)₂SO₄, [Ag(NH₃)₂]⁺, [Cu(NH₃)₄]²⁺ or 450 °C could improve the adsorption abilities of montmorillonite for Cs⁺. However, more than 89% of adsorbed Cs⁺ on montmorillonite could be desorbed by 2 mol/L HNO₃ solutions. The XRD and SEM analysis further showed that the structure of the Cs-adsorbed or modified montmorillonite were different from that of the original one.     

Pre-concentration of naturally occurring radionuclides and the determination of (212)Pb from fresh waters

A novel technique has been developed for determining the ²¹²Pb activity of fresh waters. This is of interest to environmental monitoring programmes that utilise gross α-activity methods to screen for anthropogenic radionuclides. The contribution from ²¹²Pb varies, and is difficult to experimentally measure due to its relatively short half-life (t_½ = 10.6 h) and low environmental activity (<0.1 Bq l⁻¹). The use of a three-stage technique that encompasses a unique form of pre-concentration, separation and analysis by liquid scintillation counting allows a lower detection limit of 0.006 Bq l⁻¹ with a chemical yield of 92.5 ± 5.6%. The measurement can be obtained within 7 h of sample collection, and is calculated using the radioactive decay of ²¹²Bi. Other naturally occurring radionuclides may also be extracted using the pre-concentration stage of the technique, with efficiencies above 90% at a range of pH values.     

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.     

Radioactivity measurements in moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis) samples collected from Marmara region of Turkey

The present study was conducted to compare the ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U activity concentrations in epigeic moss (Hypnum cupressiforme) and lichen (Cladonia rangiformis). The activity levels in 37 moss and 38 lichen samples collected from the Marmara region of Turkey were measured using a gamma spectrometer equipped with a high purity germanium (HPGe) detector. The activity concentrations of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U in the moss samples were found to be in the range of 0.36-8.13, 17.1-181.1, 1.51-6.17, and 0.87-6.70 Bq kg⁻¹ respectively, while these values were below detection limit (BDL)-4.32, 16.6-240.0, 1.32-6.47, and BDL-3.57 Bq kg⁻¹ respectively in lichen. The average moss/lichen activity ratios of ¹³⁷Cs, ⁴⁰K, ²³²Th, and ²³⁸U were found to be 1.32 ± 0.57, 2.79 ± 1.67, 2.11 ± 0.82, and 2.19 ± 1.02, respectively. Very low ¹³⁷Cs concentrations were observed in moss and lichen samples compared to soil samples collected from the same locations in a previous study. Seasonal variations of the measured radionuclide activities were also examined in the three sampling stations.     

Activities of Po and Pb in the water column at Kuala Selangor, Malaysia

Natural radionuclides, such as ²¹⁰Po and ²¹⁰Pb were measured in the water samples collected from six stations at Kuala Selangor, Malaysia. Results for ²¹⁰Po and ²¹⁰Pb in dissolved and particulate phases have showed the difference in distribution and chemical behavior. The fluctuation activities of ²¹⁰Po and ²¹⁰Pb depend on wave action, geology and degree of fresh water input occurring at study areas and probably due to different sampling dates. The distribution coefficient, K_d, values of ²¹⁰Po and ²¹⁰Pb ranged from 2.0 × 10³ l g⁻¹ to 265.15 × 10⁵ l g⁻¹, and from 3.0 × 10³ l g⁻¹ to 558.16 × 10⁵ l g⁻¹, respectively. High K_d values of ²¹⁰Po and ²¹⁰Pb indicated that a strong adsorption of ²¹⁰Po and ²¹⁰Pb onto suspended particles, and the sinking of both nuclides on the seabed at study locations were controlled by the characteristics of suspended particles.     

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.     

Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Vertical distributions of (99)Tc and the (99)Tc/(137)Cs activity ratio in the coastal water off Aomori, Japan

Using a sector-field ICP-MS the vertical distributions of the ⁹⁹Tc concentration and ⁹⁹Tc/¹³⁷Cs activity ratio were measured in the coastal waters off Aomori Prefecture, Japan, where a spent-nuclear-fuel reprocessing plant has begun test operation. The ⁹⁹Tc concentrations in surface water ranged from 1.8 to 2.4 mBq/m³, no greater than the estimated background level. Relatively high ⁹⁹Tc/¹³⁷Cs activity ratios (10-12 × 10⁻⁴) would be caused by the inflow of the high-⁹⁹Tc/¹³⁷Cs water mass from the Japan Sea. There is no observable contamination from the reprocessing plant in the investigated area. The ⁹⁹Tc concentration and the ⁹⁹Tc/¹³⁷Cs activity ratio in water column showed gradual decreases with depth. Our results implied that ⁹⁹Tc behaves in a more conservative manner than ¹³⁷Cs in marine environments.     

Vertical distribution of anthropogenic radionuclides in cores from contaminated floodplains of the Yenisey River

The Mining and Chemical Industrial Combine, Zheleznogorsk (MCIC, previously known as Krasnoyarsk-26) on the River Yenisey has contaminated the surrounding environment with anthropogenic radionuclides as a result of discharges of radioactive wastes. The purpose of this study was to investigate the vertical distribution of anthropogenic contamination (¹³⁷Cs and plutonium) within floodplain areas at different distances from the discharge point. Sites were chosen that display different characteristics with respect to periodic inundation with river water. Cs-137 activity concentrations were in the range 23–3770 Bq/kg (dry weight, d.w.); Pu-239,240 activity concentrations were in the range <0.01–14.2 Bq/kg (d.w.). Numerous sample cores exhibited sub-surface maxima which may be related to the historical discharges from the MCIC. Possible evidence indicating the deposition of earlier discharges at MCIC in deeper core layers was observed in the ²³⁸Pu:^239,240Pu activity ratio data: a Pu signal discernible from global fallout could be observed in numerous samples. Cs-137 and Pu-239,240 activity concentrations were correlated with the silt fraction (% by mass <63 μm) though no significant correlation was observed between (grain-size) normalised ¹³⁷Cs activity concentrations and distance downstream from the MCIC.     

Intake of ²³⁸U and ²³²Th through the consumption of foodstuffs by tribal populations practicing slash and burn agriculture in an extremely high rainfall area

The concentration of naturally occurring radionuclides ²³²Th, ²³⁸U was determined using Instrumental Neutron Activation Analysis (INAA) in different food groups namely cereals, vegetables, leafy vegetables, roots and tubers cultivated and consumed by tribal population residing around the proposed uranium mine. The study area is a part of rural area K. P. Mawthabah (Domiasiat) in the west Khasi Hills District of Meghalaya, India located in the tropical region of high rainfall that remains steeped in tribal tradition without much outside influence. Agriculture by Jhum (slash and burn) cultivation and animal husbandry are the main occupation of the tribal populations. A total of 89 samples from locally grown food products were analyzed. The concentration of ²³⁸U and ²³²Th in the soil of the study area was found to vary 1.6-15.5 and 2.0-5.0 times respectively to the average mean value observed in India. The estimated daily dietary intake of ²³⁸U and ²³²Th were 2.0 μg d⁻¹ (25 mBq d⁻¹) and 3.4 μg d⁻¹ (14 mBq d⁻¹) is comparable with reported range 0.5-5.0 μg d⁻¹ and 0.15-3.5 μg d⁻¹ respectively for the Asian population.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

Several natural and anthropogenic radionuclides (²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of ²¹⁰Pb was 126 Bq m⁻² a⁻¹, very close to the flux of northern hemisphere average (125 Bq m⁻² a⁻¹). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.     

Migration of Cs and Sr in undisturbed soil profiles under controlled and close-to-real conditions

Migration of ¹³⁷Cs and ⁹⁰Sr in undisturbed soil was studied in large lysimeters three and four years after contamination, as part of a larger European project studying radionuclide soil–plant interactions. The lysimeters were installed in greenhouses with climate control and contaminated with radionuclides in an aerosol mixture, simulating fallout from a nuclear accident. The soil types studied were loam, silt loam, sandy loam and loamy sand. The soils were sampled to 30–40 cm depth in 1997 and 1998. The total deposition of ¹³⁷Cs ranged from 24 to 45 MBq/m², and of ⁹⁰Sr from 23 to 52 MBq/m². It was shown that migration of ¹³⁷Cs was fastest in sandy loam, and of ⁹⁰Sr fastest in sandy loam and loam. The slowest migration of both nuclides was found in loamy sand. Retention within the upper 5 cm was 60% for both ¹³⁷Cs and ⁹⁰Sr in sandy loam, while in loamy sand it was 97 and 96%, respectively. In 1998, migration rates, calculated as radionuclide weighted median depth (migration centre) divided by time since deposition were 1.1 cm/year for both ¹³⁷Cs and ⁹⁰Sr in sandy loam, 0.8 and 1.0 cm/year, respectively, in loam, 0.6 and 0.8 cm/year in silt loam, and 0.4 and 0.6 cm/year for ¹³⁷Cs and ⁹⁰Sr, respectively, in loamy sand. A distinction is made between short-term migration, caused by events soon after deposition and less affected by soil type, and long-term migration, more affected by e.g. soil texture. Three to four years after deposition, effects of short-term migration is still dominant in the studied soils.     

Inventory and vertical migration of ¹³⁷Cs in Spanish mainland soils

In this study the total activity of ¹³⁷Cs deposited per unit area over the Spanish peninsular territory was analysed using a 150 × 150 km² mesh grid, with samples taken from 29 points. The deposited activities ranged between 251 and 6074 Bq/m². A linear relationship was obtained between these values and the mean annual rainfall at each sampling point which allowed a map to be drawn, using GIS software, which shows the distribution of total deposited ¹³⁷Cs activity across the Spanish mainland. At twelve of these sampling points the vertical migration profile of ¹³⁷Cs was obtained. These profiles are separated into two groups with different behaviour, one of which includes clay and loam soils and the other containing sandy soils. For both groups of profiles the parameters of the convective-diffusive model, which describes the vertical migration of ¹³⁷Cs in the soil, v (apparent convection velocity) and D (apparent diffusion coefficient) were calculated.