Thermal neutron fluence from ultra low-level gamma-ray spectrometry of spoons activated during the JCO criticality accident at Tokai-mura in 1999

During the JCO-accident in Tokai-mura in 1999, the surrounding village was irradiated by an uncontrolled neutron flux. At some locations in that village, the thermal neutron flux was determined retrospectively by measurement of the very low activity of 51Cr and 60Co in stainless-steel spoons using gamma-ray spectrometry in underground laboratories. Activities determined in the HADES underground facility are presented here, together with calibrations performed using a well-defined thermal neutron flux to directly estimate the fluence of thermal neutrons independent of most assumptions. The results show measurable 51Cr in three samples and 60Co in four samples taken from locations at distances of up to 430m from the accident location despite the elapse of 4 half-lives of 51Cr before measurement. Effects of air transport of the samples were considered and shown to be negligible.     

Measurements of 60Co in spoons activated by neutrons during the JCO criticality accident at Tokai-mura in 1999

Neutron activated items from the vicinity of the place where the JCO criticality accident occurred have been used to determine the fluence of neutrons around the facility and in nearby residential areas. By using underground laboratories for measuring the activation products, it is possible to extend the study to also cover radionuclides with very low activities from long-lived radionuclides. The present study describes gamma-ray spectrometry measurements undertaken in a range of underground laboratories for the purpose of measuring (60)Co more than 2 years after the criticality event. The measurements show that neutron fluence determined from (60)Co activity is in agreement with previous measurements using the short-lived radionuclides (51)Cr and (59)Fe. Limits on contamination of the samples with (60)Co are evaluated and shown to not greatly affect the utility of neutron fluence determinations using (60)Co activation.     

Fate of Co at a sludge land application site

Vertical distributions of ⁶⁰Co are determined in soil cores obtained from a 10-ha grassland, where anaerobically digested sludge was applied by surface spraying from 1986 to 1995 on the U.S. Department of Energy's Oak Ridge Reservation. These results, along with historical application records, are used to estimate vertical-migration rates and perform a mass balance. The presence of ⁶⁰Co results solely from the sludge-application process. Soil, vegetation, and surface-water samples were collected. Eleven soil cores were sectioned into 3-cm increments and analyzed by gamma-ray spectrometry. No ⁶⁰Co was detected in the vegetation or water samples. The downward migration rate of ⁶⁰Co in the upper 15 cm of soil ranged from 0.50 to 0.73 cm/yr. About 98%, 0.020 ± 0.011 Bq/cm², of ⁶⁰Co remained in the upper 15 cm of soil, which compared favorably with the expected ⁶⁰Co activity based on historical records of 0.019 ± 0.010 Bq/cm².     

Depth profile of ²³⁶U/²³⁸U in soil samples in La Palma, Canary Islands

The vertical distribution of the ²³⁶U/²³⁸U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the ²⁴⁰Pu/²³⁹Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA^® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios ²³⁶U/²³⁸U, ²⁴⁰Pu/²³⁹Pu and ²³⁶U/²³⁹Pu, respectively. The ²³⁶U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated a global fallout signature we assume the same origin as the probable source for ²³⁶U. Our measured ²³⁶U/²³⁹Pu value of around 0.2 is within the expected range for this contamination source.     

Laboratory studies of the diffusive transport of Cs and Co through potential waste repository soils

Tests using reconstituted samples have been performed to assess the diffusive transport of ¹³⁷Cs and ⁶⁰Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D_e) and sorption coefficients (K_d) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D_e values obtained in this study were of the order of 10⁻⁶ cm² s⁻¹ for both species, higher than previously published data. The K_d values from the diffusion and batch sorption tests were in reasonable agreement for ¹³⁷Cs, but an order of magnitude different for ⁶⁰Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.     

Cs,Co and K uptake by lettuce plants in two distributions of soil contamination

¹³⁷Cs and ⁶⁰Co, two of the radionuclides more representative of discharges from nuclear facilities, are of interest for radiological protections because of their great mobility in biosphere and affinity with biological systems. The aim of the present work is the investigation of the possible influence of the vertical distribution of ¹³⁷Cs and ⁶⁰Co in soil upon their uptake by lettuce as function of plant's growth. An experiment ad hoc has been carried out in field conditions. The results show that (i) the transfer of ¹³⁷Cs and ⁶⁰Co from soil to lettuce is independent by their distribution in soil, (ii) the soil–plant transfer factors of ¹³⁷Cs and ⁶⁰Co show a similar trend vs. growth stage, (iii) the ⁴⁰K transfer factor trend is different from those of anthropogenic radionuclides, and (iv) ¹³⁷Cs and ⁶⁰Co specific activities are about 1 Bq/kg, in the mature vegetable with soil activity from 9 to 21 kBq/m².     

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.     

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.     

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.     

Time-series sampling of Ra and Ra at the inlet to Great South Bay (New York): a strategy for characterizing the dominant terms in the Ra budget of the bay

Ra isotopes are a powerful tool for quantifying the flux of submarine groundwater discharge (SGD) into the sea. Previous studies of ²²³Ra and ²²⁴Ra mass balances in coastal embayments have shown that the Ra balance is dominated by supply via SGD, exchange with the open ocean and radioactive decay. The current study shows that a single time series over a tidal cycle at the principal inlet to Great South Bay (NY, US) is sufficient to determine the net flux of Ra across the inlet, and also can be used to estimate the decay of short-lived Ra in the bay. Estimates of the net Ra flux obtained from a single tidal time-series by using three different approaches agree with those determined from a more time-consuming survey of Ra within the bay, and may represent a first step of estimating SGD in bays and coastal lagoons.     

137Cs in marine samples from the Brazilian southeastern coastal region

The present work presents the results of ¹³⁷Cs concentration in seawater, fish and sediments samples collect in 11 sampling points, crossing the Brazilian Southeastern coastal region, from Vitória (ES) to Santos (SP), on a routine basis from 1997 to 2002. This monitoring program was carried out by the Instituto de Radioproteção e Dosimetria (IRD/CNEN/MCT), in cooperation with the Instituto de Estudos do Mar Almirante Paulo Moreira (IEAPM/Brazilian Navy), aiming at determining artificial radionuclides in marine samples. Additionally to the ¹³⁷Cs results, ⁹⁰Sr concentrations in fish samples from 1998 to 2002 are also reported.The ¹³⁷Cs in seawater follows a lognormal distribution, with a geometric mean of 1.8 Bq m^-3 and a geometric standard deviation of 1.4 (n=54), decay corrected to June/2002. For ¹³⁷Cs levels in fish samples a geometric mean of 0.19 Bq kg⁻¹ and a geometric standard deviation of 2.9 (n=39), decay corrected to June/2002, with a range of 0.03 to 1.7 Bq kg⁻¹, were obtained. Based on the ¹³⁷Cs mean concentration in fish as well as in seawater, a transfer factor of 1 × 10² was calculated, which is quite in agreement with the recommended value found in the Safety Report Serie 19.     

Nationwide indoor 222Rn and 220Rn map for India: a review

Considering the role of radon in epidemiology, an attempt was made to make a nation-wide map of indoor ²²²Rn and ²²⁰Rn for India. More than 5000 measurements have been carried out in 1500 dwellings across the country comprising urban and nonurban locations. The solid state nuclear track detectors based twin cup ²²²Rn/²²⁰Rn discrimination dosimeters were deployed for the measurement of indoor ²²²Rn, ²²⁰Rn and their progeny levels. The geometric means of estimated annual inhalation dose rate due to indoor ²²²Rn, ²²⁰Rn and their progeny in the dwellings was 0.94 mSvy⁻¹ (geometric standard deviation 2.5). It was observed that the major contribution to the indoor inhalation dose was due to indoor ²²²Rn and its progeny. However, the contribution due to indoor ²²⁰Rn and its progeny was not trivial as it was found to be about 20% of the total indoor inhalation dose rates. The indoor ²²²Rn levels in dwellings was significantly different depending on the nature of walls and floorings.     

Aspects on the analysis of 210Po

There has been little development regarding analysis of polonium (Po) in environmental samples since the 1960ies. This is due to the straightforward spontaneous deposition of this element on silver (Ag), nickel (Ni) or copper (Cu) without any radiochemical separation. For many years, no radiochemical yield determinant was used and it was generally supposed that the yield was 100% after two depositions. Counting was often done using ZnS scintillation counter coupled to a photomultiplier tube. However, the use of the yield determinants ²⁰⁸Po and ²⁰⁹Po and the development of alpha spectrometry showed that the yield was lower. Furthermore, the tendency of Po to volatilize at low temperatures constrains the sample preparation techniques; dry-ashing cannot be used. But during the wet-ashing procedure, there are still some losses.The aim of this study was to evaluate the Po losses during wet-ashing by the use of a double-tracer technique. We have found that the losses were about 30% when open glass beakers were used and about 17% when the samples were digested in microwave oven. When long-necked bottles (Kjeldahl flasks) were used, a loss of about 20% was registered.It has also been observed that ²¹⁰Pb to some extent is plating out together with its daughter nuclide Po during the electrochemical deposition. This will result in a systematic error since an unknown amount of supported ²¹⁰Po will be produced from the ²¹⁰Pb decay depending on the fraction of ²¹⁰Pb being deposited on the disc and the waiting time between deposition and measurement of the sample. A further consequence of this is that in the assessment of the ²¹⁰Pb content in the sample, very often the remaining liquid is stored after deposition for build-up of ²¹⁰Po. Since some ²¹⁰Pb is lost on the disc, the result for ²¹⁰Pb will be too low. Both these systematic errors give rise to a too high ²¹⁰Po/²¹⁰Pb ratio. The fraction of ²¹⁰Pb which is plating out has been assessed in this study for different matrices and is about 50-90%. During the measurement by solid state Si-detectors, some Po is evaporated in the vacuum conditions contaminating the detectors. Experiments have here been done by heating the discs after deposition which indicate that less Po is evaporated from Ag than from Ni. The losses from Ag are less than that from the other metals probably due to a deeper penetration into the surface of Po. We conclude that in most aspects, Ag is better to use than the other plating metals.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

The effect of air mass origin on the ambient concentrations of Be and Pb in Islamabad, Pakistan

Concentration of radionuclides ²¹⁰Pb and ⁷Be, having half lives of 22.3 years and 53.29 days, respectively, in the surface air samples of Islamabad (33.38° N, 73.10° E and Altitude ∼536 m asl.) are measured. The non-destructive technique of gamma-spectrometry, with a high purity germanium HPGe detector, was employed for the analysis of all samples. The annual average concentrations of ²¹⁰Pb and ⁷Be in the surface air samples were determined as 0.284 ± 0.15 and 3.171 ± 1.14 mBq m⁻³, respectively. Our results have shown a seasonal variation of the concentration of ⁷Be in air samples with high values for the spring season. High concentrations for ²¹⁰Pb are obtained when air masses originate from plain areas of Pothohar region, located in the South-West, West and North West of Islamabad. Our values of concentrations show a nice agreement with the relevant reported results.     

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.     

Determination of U, Pu and Am isotopes in Irish Sea sediment by a combination of AMS and radiometric methods

Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA^® and finally Am separation with TRU^® Resin.Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of ²³⁶U/²³⁸U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.     

Transfer factors of Polonium from soil to parsley and mint

Transfer factors of ²¹⁰Po from soil to parsley and mint have been determined. Artificial polonium isotope (²⁰⁸Po) was used as a tracer to determine transfer factor of Po from soil to plant in pot experiments. Two plant growing systems were used for this study namely, an outdoor system and a sheltered system by a polyethylene tent. ²⁰⁸Po and ²¹⁰Po were determined in soil and different parts of the studied plants (stem and leaf), using alpha spectroscopy. The results have shown that there was a clear uptake of ²⁰⁸Po by roots to leaves and stems of both plants. Higher values of transfer factors using the ²¹⁰Po activity concentrations than the ²⁰⁸Po activity concentration were observed. Transfer factors of ²¹⁰Po from soil to parsley varied between 20 × 10⁻² and 50 × 10⁻² and 22 × 10⁻³ and 67 × 10⁻³ in mint, while ²⁰⁸Po transfer factors varied between 4 × 10⁻² and 12 × 10⁻² for parsley and 10 × 10⁻² and 22 × 10⁻² in mint. Transfer factors of Po were higher in those plants grown in the sheltered system than in the open system; about 75% of Po was transferred from atmosphere to parsley parts using the two systems. Ratios of transferred Po from soil to mint stem and leaf in the sheltered system were higher by 2 times from those in the open system.     

Adsorption models of Cs radionuclide and Sr (II) on some Egyptian soils

Distribution of cesium (¹³⁴Cs and ¹³⁷Cs) and strontium (Sr-II) between soil/water phases depends on many factors such as concentration of these ions between phases, the cation exchange capacity (CEC) of the soil as well as its clay content, chemical composition (especially Na, K, Ca, and Mg ions), grain size distribution, calcite, iron oxide content, and organic coatings. Distribution coefficients (Kd) of cesium (labeled with ¹³⁷Cs) and strontium were measured on the grain size distributions ≥32 μm of four soil samples. These soils were obtained from four different locations within Inshas site in Egypt and three groundwater samples were obtained from the same site locations. X-ray diffraction showed that the soil samples consisted mainly of quartz mixed with the minor amounts of kaolonite and clay minerals. Sorption experiments were carried out at strontium aqueous concentrations range 10⁻⁷ to 10⁻⁴ mol l⁻¹. The CEC and Kds for cesium and strontium were measured at the same metal concentrations range. Distribution coefficients of cesium were found to be influenced by the composition of the soil, while the distribution coefficients of strontium were found to depend on calcium concentrations in the soil/groundwater system. The aim of this study was to determine the safety assessment of disposal ¹³⁷Cs radionuclide and Sr(II) in the aquifer regions inside the Inshas site. Sequential extraction tests showed that, strontium was associated with the carbonate fractions and majority of cesium was sorbed on the iron oxides and the residue.