Determination of radionuclide levels in rainwater using ion exchange resin and gamma-spectrometry.

The evaluation of radioactivity accidentally released into the atmosphere involves determining the radioactivity levels of rainwater samples. Rainwater scavenges atmospheric airborne radioactivity in such a way that surface contamination can be deduced from rainfall rate and rainwater radioactivity content. For this purpose, rainwater is usually collected in large surface collectors and then measured by gamma-spectrometry after such treatments as evaporation or iron hydroxide precipitation. We found that collectors can be adapted to accept large surface (diameter 47mm) cartridges containing a strongly acidic resin (Dowex AG 88) which is able to quantitatively extract radioactivity from rainwater, even during heavy rainfall. The resin can then be measured by gamma-spectrometry. The detection limit is 0.1Bq per sample of resin (80g) for (137)Cs. Natural (7)Be and (210)Pb can also be measured and the activity ratio of both radionuclides is comparable with those obtained through iron hydroxide precipitation and air filter measurements. Occasionally (22)Na has also been measured above the detection limit. A comparison between the evaporation method and the resin method demonstrated that 2/3 of (7)Be can be lost during the evaporation process. The resin method is simple and highly efficient at extracting radioactivity. Because of these great advantages, we anticipate it could replace former rainwater determination methods. Moreover, it does not necessitate the transportation of large rainwater volumes to the laboratory.

A comparison of alpha and gamma spectrometry for environmental natural radioactivity surveys.

An alpha-spectrometry, using automated borate fusion and sequential extraction and exchange chromatography, was used to determine the uranium and thorium based on environmental radioactivity of 20 soil samples. The same set of the samples was analysed using gamma-spectrometry with an HPGe detector. The two data sets were checked for coherence using Z-score and chi2 statistical tests. We show that gamma-spectrometry is a valid alternative to time-consuming alpha-spectrometry for the determination of natural uranium and thorium activity in soil (activity range: 12.5-58.2 Bq/kg). The measured activities were compared with the theoretical activities to ensure secular equilibrium in the 238U and 232Th series. For 226Ra, a special study was made on deconvolution of the 186 keV multiplet with the Levenberg-Marquardt algorithm. Finally, the combined use of Z-score and chi2-tests was found to be a powerful tool for comparing the results obtained with two different methods.

Gamma spectrometry and gamma and X-ray tomography of nuclear fuel

The purpose of gamma spectrometry and gamma and X-ray tomography of nuclear fuel is to determine both radionuclide concentration and integrity and deformation of nuclear fuel. The aims of this thesis have been to find out the basics of gamma spectrometry and tomography of nuclear fuel, to find out the operational mechanisms of gamma spectrometry and tomography equipment of nuclear fuel, and to identify problems that relate to these measurement techniques. In gamma spectrometry of nuclear fuel the gamma-ray flux emitted from unstable isotopes is measured using high-resolution gamma-ray spectroscopy. The production of unstable isotopes correlates with various physical fuel parameters. In gamma emission tomography the gamma-ray spectrum of irradiated nuclear fuel is recorded for several projections. In X-ray transmission tomography of nuclear fuel a radiation source emits a beam and the intensity, attenuated by the nuclear fuel, is registered by the detectors placed opposite. When gamma emission or X-ray transmission measurements are combined with tomographic image reconstruction methods, it is possible to create sectional images of the interior of nuclear fuel. MODHERATO is a computer code that simulates the operation of radioscopic or tomographic devices and it is used to predict and optimise the performance of imaging systems. Related to the X-ray tomography, MODHERATO simulations have been performed by the author. Gamma spectrometry and gamma and X-ray tomography are promising non-destructive examination methods for understanding fuel behaviour under normal, transient and accident conditions.

Activity concentrations of radionuclides in 5 short cores taken in 2007-2008 measured by ICP-MS and HPGe gamma spectrometry

Natural radionuclides and man-made 137Cs were analyzed in five short sediment cores taken in northern part of the Gulf of Eilat (Gulf of Aqaba) in order to provide information on sedimentation and mixing rates and sediment sources. The maximum estimates of sedimentation rates based on excess 210Pb were found to vary between 0.105 ± 0.020 and 0.35 ± 0.23 cm · year**-1. Even the lowest estimates are significantly higher than those expected from dust deposition, suggesting other sources and processes being responsible for most of the allochthonous material accumulation, including periodical floods following heavy rain events, internal erosion or triggers, like earthquakes. In 137Cs depth profiles no 1963 related nuclear weapon test maxima were found; instead, the activities decrease monotonically, suggesting that a major process leading to radionuclides' depth distribution might be mixing. The mixing rates calculated from 137Cs, excess 210Pb and excess 228Th reach values up to 2.18 ± 0.69 cm**2 · year**-1.

Assessment of the environmental radiation by in situ gamma ray spectrometry

Naturally occurring radioactive materials (NORM) under certain conditions can reach hazardous radiological levels contributing to an additional exposure dose to ionizing radiation. Most environmental concerns are associated with uranium mining and milling sites, but the same concerns should be addressed to natural near surface occurrences of uranium as well as man-made sources such as technologically enhanced naturally occurring radioactive materials (TENORM) resulting from phosphates industry, ceramic industry and energy production activities, in particular from coal-fired power plants which is one of the major sources of increased exposure to man from enhanced naturally occurring materials. This work describes the methodology developed to assess the environmental radiation by in situ gamma spectrometry in the vicinity of a Portuguese coal fired power plant. The current investigation is part of a research project that is undergoing in the vicinity of Sines Coal-Fired Power Plant (south of Portugal) until the end of 2013.

Radioactivity levels of 238U and 232Th decay series and related dose rates in the surroundings of a coal power plant using high resolution g-spectrometry

Gamma radiations measurements were carried out in the vicinity of a coal-fired power plant located in the southwest coastline of Portugal. Two different gamma detectors were used to assess the environmental radiation within a circular area of 20 km centred in the coal plant: a scintillometer (SPP2 NF, Saphymo) and a high purity germanium detector (HPGe, Canberra). Fifty urban and suburban measurements locations were established within the defined area and two measurements campaigns were carried out. The results of the total gamma radiation ranged from 20.83 to 98.33 counts per second (c.p.s.) for both measurement campaigns and outdoor doses rates ranged from 77.65 to 366.51 Gy/h. Natural emitting nuclides from the U-238 and Th-232 decay series were identified as well as the natural emitting nuclide K-40. The radionuclide concentration from the uranium and thorium series determined by gamma spectrometry ranged from 0.93 to 73.68 Bq/kg, while for K-40 the concentration ranged from 84.14 to 904.38 Bq/kg. The obtained results were used primarily to define the variability in measured environmental radiation and to determine the coal plant’s influence in the measured radiation levels. The highest values were measured at two locations near the power plant and at locations between the distance of 6 and 20 km away from the stacks, mainly in the prevailing wind direction. The results showed an increase or at least an influence from the coal-fired plant operations, both qualitatively and quantitatively.

As técnicas NASVD e MNF e sua aplicação na redução de ruídos em dados gamaespectrométricos

A desintegração radioativa é um processo aleatório e a estimativa de todas as medidas associadas é governada por leis estatísticas. Os perfis de taxas de contagem são sempre "ruidosos" quando utilizados períodos curtos como um segundo para cada medida. Os filtros utilizados e posteriormente as correções feitas no processamento atual de dados gamaespectrométricos não são suficientes para remover ou diminuir, consideravelmente, o ruído oriundo do espectro. Dois métodos estatísticos que atuam diretamente nos dados coletados, isto é, nos espectros, vêm sendo sugeridos na literatura para remover e minimizar estes ruídos remanescentes o Noise-Adjusted Singular Value Decomposition - NASVD e Maximum Noise Fraction - MNF. Estes métodos produzem uma redução no ruído de forma significativa. Neste trabalho eles foram implementados dentro do ambiente de processamento do software Oasis Montaj e aplicados na área compreendida pelos blocos I e II do levantamento aerogeofísico que recobre a porção oeste da Província Mineral do Tapajós, entre os Estados do Pará e Amazonas. Os dados filtrados e não-filtrados com as técnicas de NASVD e MNF foram processados com os parâmetros e constantes fornecidos pela empresa Lasa Engenharia e Prospecções S.A., sendo estes comparados. Os resultados da comparação entre perfis e mapas apresentaram-se de forma promissora, pois houve um ganho na resolução dos produtos.

Radiation dose rates and exposure associated to Technologically Enhanced Naturally Occurring Radioactive Materials (TENORM) at locations of a Portuguese coal-fired power plant

Coal contains trace quantities of natural radionuclides such as Th-232, U-235, U-238, as well as their radioactive decay products and 40K. These radionuclides can be released as fly ash in atmospheric emissions from coal-fired power plants, dispersed into the environment and deposited on the surrounding top soils. Therefore, the natural radiation background level is enhanced and consequently increase the total dose for the nearby population. A radiation monitoring programme was used to assess the external dose contribution to the natural radiation background, potentially resulting from the dispersion of coal ash in past atmospheric emissions. Radiation measurements were carried out by gamma spectrometry in the vicinity of a Portuguese coal-fired power plant. The radiation monitoring was achieved both on and off site, being the boundary delimited by a 20 km circle centered in the stacks of the coal plant. The measured radionuclides concentrations for the uranium and thorium series ranged from 7.7 to 41.3 Bq/kg for Ra-226 and from 4.7 to 71.6 Bq/kg for Th-232, while K-40 concentrations ranged from 62.3 to 795.1 Bq/kg. The highest values were registered near the power plant and at distances between 6 and 20 km from the stacks, mainly in the prevailing wind direction. The absorbed dose rates were calculated for each sampling location: 13.97-84.00 ηGy/h, while measurements from previous studies carried out in 1993 registered values in the range of 16.6-77.6 ηGy/h. The highest values were registered at locations in the prevailing wind direction (NW-SE). This study has been primarily done to assess the radiation dose rates and exposure to the nearby population in the surroundings of a coal-fired power plant. The results suggest an enhancement or at least an influence in the background radiation due to the coal plant past activities.

Brazil nuts: determination of natural elements and aflatoxin

A study was carried out to evaluate the association of levels of radioactivity, selenium and aflatoxin in shelled Brazil nuts, which were classified in different sizes, for export. The selenium determinations were performed by inductively coupled plasma optical emission spectrometry (LOQ = 3.0 µg g-1), and aflatoxins were detected by Liquid chromatography-mass spectrometry (LOQ = 0.85 µg kg-1), recovery rates were between 92 and 100%. Radioactivity was measured by high-resolution gamma spectrometry. The selenium mean concentration was (22.7 ± 7.4) µg g-1. (n = 30). Mean activities determined for the following radium isotopes were: 15.77 Bq kg-1 for 224Ra, 104.8 Bq kg-1 for 226Ra and 99.48 Bq kg-1 for 228Ra. For 226Ra, the levels did not vary significantly with nut sizes, although such differences were observed for 224Ra and 228Ra. There was no statistically significant association between the level of selenium and the activity of radionuclides, however, there was correlation between the radionuclides. Aflatoxins above the quantification limit were not found.

Transfer of radionuclides from soil to vegetation in selected Irish ecosystems

This thesis details the findings of a study relating the transfer of 238U, 228Ra (232Th), 226Ra, and 137Cs from soil to vegetation in an Atlantic blanket bog, upland blanket bog and semi-natural grassland situated along the north-west coast of Ireland. The results of this study provide information on the uptake of these radionuclides by the indigenous vegetation found present in these ecosystems. The ecosystems chosen are internationally recognizable ecosystems and provide a wide variety of vegetation species and contrasting soil physiochemical properties which allow the influence of these parameters on radionuclide uptake to be assessed. The levels of radionuclides in the soil and vegetation were measured using gamma spectrometry, alpha spectrometry and ICP-MS. The nutrient status of the vegetation and soil physiochemical properties were measured using atomic absorption, flame photometry and other analytical techniques. The results of the study indicate that the uptake of 238U and 228Ra (232Th) by vegetation from all three ecosystems was negligible as the levels in all vegetation was below the limits of detection for the methods used in this study. These results appear to indicate that the vegetation studied do not possess the ability to accumulate significant levels of these radionuclides however this assumption cannot be upheld in the case of the Atlantic blanket bog as the levels in the soil of this ecosystem were too low for detection. Similar results were obtained for 226Ra uptake in both the Atlantic blanket bog and grassland for all vegetation with the exception of H. lanatus from the grassland ecosystem. Radium-226 uptake in upland blanket bog was higher and was detectable in the majority of vegetation indigenous to this ecosystem. Transfer factor values ranged from 0.07 to 2.35 and the TF values for E. tetralix were significantly higher than all other vegetation studied. This species of heather demonstrated the ability to accumulate 226Ra to a greater extent than all other vegetation. The uptake of 226Ra by upland blanket bog vegetation appears to be significantly influenced by a range of soil physiochemical properties. The nutrient status of the vegetation, in particular the calcium content in the vegetation appears to have a negative impact on the uptake of this radionuclide. Potassium-40 was detectable in all vegetation present in the three ecosystems and the levels in the grassland soil were significantly higher than the levels in both bogland soils. Transfer factor values for Atlantic blanket bog vegetation ranged from 0.9 to 13 .8 and were significantly higher in E. vaginatum in comparison to C. vulgaris. Potassium-40 TF values for upland blanket bog vegetation on average ranged from 1.4 for C. vulgaris (stems) to 5.2 for E. vaginatum and were statistically similar for all species of vegetation. Transfer factor values for grassland vegetation ranged from 0.7 to 3.8 and were also statistically similar for all species of vegetation indicating that the transfer of 40K to vegetation within the upland bog and grassland ecosystem is not dependent on plant species. Comparisons of 40K TF values for all three ecosystems indicate that the uptake in E. vaginatum from the Atlantic blanket bog was statistically higher than all other vegetation studied. This appears to indicate that E. vaginatum has the ability to accumulate 40K, however, this species of vegetation was also present in the upland blanket and did not demonstrate the same behaviour. The uptake of 40K by vegetation from all three ecosystems was significantly affected by a range of soil physiochemical properties and in some cases the results were contradictory in nature possibly indicating that the affect of these parameters on 40K uptake is species dependent. The most obvious trend in the data was the influence of soil CEC and magnesium levels in vegetation on 40K TF values. A positive correlation was apparent between the CEC of the soil and 40K uptake in vegetation from both the Atlantic blanket bog and grassland ecosystem. A similar trend was apparent between magnesium levels in vegetation and 40K TF values for the upland blanket bog and grassland vegetation. Caesium-13 7 levels were found to be significantly higher in the two bogland soils in comparison to the grassland soil and levels of 137Cs decreased with increasing soil depth. Transfer factor values for Atlantic blanket bog vegetation ranged from 1.9 to 9.6 and TF values were significantly higher in the leaves o f C. vulgaris in comparison to all other vegetation from this ecosystem. Caesium-13 7 TF values for the upland blanket bog vegetation on average ranged from 0.29 for E. tetralix to 1.6 for C. vulgaris. Uptake by the leaves of C. vulgaris was significantly higher than all other vegetation present thereby supporting the trend found within the Atlantic blanket bog vegetation. These results appear to indicate that the leaves of C. vulgaris have the ability to accumulate significant quantities of 137Cs and also that the uptake of 137Cs by this vegetation is dependent on plant compartment as the stems of this vegetation contained significantly lower levels than the leaves in both ecosystems. The uptake of 137Cs by grassland vegetation was very low and was only detectable in a fraction of the vegetation sampled. Caesium-137 TF values for grassland vegetation were in general lower than 0.02. The impact of soil physiochemical properties and nutrient status of vegetation on 137Cs uptake by vegetation appears to be complex and in some cases contradictory. The most apparent trend in the data was the positive influence of vegetation nutrients on 137Cs uptake in particular the magnesium levels present in the vegetation and to a lesser extent the calcium levels present. The results in general indicate that the uptake of 226Ra, 40K and 137Cs by the chosen vegetation is varied and complex and is significantly dependent on the species of vegetation, soil radionuclide concentration, soil physiochemical properties and the nutrient status of the vegetation.

Radiological impact of phosphogypsum surface application in a no-till system in Southern Brazil

The objective of this work was to determine the impact of phosphogypsum application on 226Ra and 228Ra activities in the soil and on their accumulation in soybean grains. A field experiment was carried out in Paraná state, Brazil, on a loamy Typic Hapludox, under no-till system, with increasing phosphogypsum rates: 4, 8, and 12 Mg ha-1. GammA ray spectrometry was carried out using HPGe detectors with 45 and 10% relative efficiencies, for soybean grains and soil, respectively. No increment of 226Ra and 228Ra activities was observed due to the increase in phosphogypsum rates in the soil, and a small reduction was noticed in the grains. Average values found for 226Ra and 228Ra activities were 37 and 57 Bq kg-1 in the soil and 1.44 and 3.19 Bq kg-1 in soybean grains. The application of phosphogypsum for no-till soybean production is a safe practice regarding the risks of radiation damage to human health