Alpha Spectrometric Measurements Research Articles

Distribution and transfer of naturally occurring radionuclides and 137Cs in the freshwater system of the Plitvice Lakes, Croatia, and related dose assessment to wildlife by ERICA Tool.

The aim of this study was to investigate the natural radioactivity of Plitvice Lakes, under the assumption that due to its status as a National Park, the area can be considered an example of a natural freshwater system. Also, considering the transfer parameter data as the largest source of uncertainty in radiological risk assessments, the impact of site-specific data on dose rate assessment, as opposed to currently available data, was investigated. The study included gamma and alpha spectrometric measurements of 238U, 226Ra, 210Pb, 228Ra, and 40K in water, sediment, and fish samples, as well as 137Cs due to the coinciding of the study with the Fukushima accident. The content of naturally occurring radionuclides significantly varied in sediments of different Lakes, probably as a reflection of the different underlying geology of the area. Also, the 210Pb distribution in sediments indicated an up to 312 Bq kg-1 of the allochthonous contribution of this radionuclide at the beginning of the Lake's watercourse, which probably entered into the lake system by the major inlet river with its steady decrease along downstream lakes. Low 40K activity concentrations (27.5 ± 20.1 mBq L-1) in the Lake's waters might be one of the causes of increased 137Cs activity concentrations in fish samples (1.5 ± 0.4 Bq kg-1), which was found to be an order of magnitude higher than average values for different fish species from other Croatian freshwater systems (0.2 ± 0.1 Bq kg-1). A temporary increase of 137Cs activity concentrations was measured in water samples collected immediately after the Fukushima accident. Calculated site-specific sediment/water distribution coefficients and fish/water concentration ratios for radium and caesium were on average lower than generic ones found in the literature. Background dose rate assessments performed by the ERICA Tool indicated a profound impact of different input data on assessment results with water activity concentrations resulting in significantly higher dose rates (0.1-67 μGy h-1) in comparison to sediment activity concentrations (0.03-9 μGy h-1). An incremental dose rate due to 137Cs was found to be in the range of < 0.001-0.023 μGy h-1 which, in comparison to background dose rates, can be considered negligible.

Форми знаходження радіонуклідів у донних відкладеннях приміщення 012/7 об’єкта «Укриття»

After installation of the Arch of New Safe Confinement (NSC) into design position, precipitations intake in the underroof space of the Shelter object ceased, and water evaporation began from the unorganized accumulations of radioactively contaminated water. As a result of physical and chemical processes of coagulation and deposition of sparingly soluble salts, bottom sediments, containing uranium and radionuclides, formed. The aim of the work is to determine speciation forms of uranium and radionuclides in the bottom sediments, which formed due to the drying out of unorganized accumulations of radioactively contaminated water in room 012/7 of the NSC – Shelter object. Results of the experimental determination of speciation forms of uranium and radionuclides 90Sr, 137Cs, 154Eu, 238Pu, 239+240Pu, 241Am and 244Cm in the bottom sediments of room 012/7 of the NSC – Shelter object are presented. An amount of water-soluble, exchangeable and acid-soluble uranium forms, fission products and transuranium elements in the bottom sediments of room 012/7 of the NSC – Shelter object was determined by the method of consecutive extractions. Content of uranium, 90Sr, 238Pu, 239+240Pu, 241Am and 244Cm in the leaching solutions and insoluble residue was determined by the ion-exchange method. 90Sr activity was determined by beta-radiometric measurements. Activity of 234,235,236,238U, 238Pu, 239+240Pu, 241Am and 244Cm was determined by alpha-spectrometric measurements of uranium, plutonium and americium sources. The concentration of uranium in the bottom sediments of room 012/7 was 1.02 ± 0.26 mg/g. Abundance content of uranium isotopes is 234U – 0.0159, 235U – 1.09, 236U – 0.192 and 238U – 98.71%. Isotope content of uranium in the bottom sediments, on the whole, corresponds to the isotope content of uranium in the irradiated fuel of the Chornobyl NPP 4th unit with an average burnup. The specific activity of 90Sr and 137Cs in the bottom sediments of room 012/7 is in the range of 6∙108−1∙109 Bq/kg. 239+240Pu and 241Am specific activity in the bottom sediments is in the range of 6∙105 – 8∙106 Bq/kg. 90Sr, 137Cs, 154Eu, 238Pu, 239+240Pu, 241Am and 244Сm radionuclides in the bottom sediments are in different physical and chemical forms, which determine their potential mobility. Mainly uranium and 137Cs in the bottom sediments of room 012/7 are in the exchangeable forms. An amount of water-soluble forms of uranium and 137Cs is about 1.5 – 3%. The main amount of 90Sr, more than 60% is in the carbonate forms, which are very soluble in weak acid medium, when pH is 4.8. More than 65% of 238Pu and 239+240Pu in the bottom sediments of room 012/7 are in the acid-soluble forms. Potential mobility of 241Am in the bottom sediments is notably higher than of plutonium in the soluble state, when pH 4.8, transfer more than 40% of 241Am. Relations of activities of radionuclides 137Cs/90Sr, 90Sr/239+240Pu, 241Am/239+240Pu and 44Cm/239+240Pu in the bottom sediments of room 012/7 differ significantly from the similar relations in the fuel containing materials of the Shelter object.

Alpha spectrometry and liquid scintillation counting for the measurement of 238Pu, 239Pu, 240Pu, 241Pu, 242Pu and age

A method for the measurement of the isotopic composition and time since last chemical separation (age) of plutonium is presented. The method includes alpha spectrometric measurement of 238Pu, 239Pu and 240Pu where the ratio of 239Pu and 240Pu was determined using spectral deconvolution, and liquid scintillation counting of 241Pu, after chemical separation of plutonium and americium. For the age determination, the 241Pu determined using liquid scintillation counting was combined with alpha spectrometric measurement of 241Am. The results of the isotopic composition were compared with certified reference materials with known isotopic composition, and the results of the age determination were compared with literature values of the separation dates.

Determination of Uranium Isotopic Ratios by Alpha Spectrometry for Nuclear Materials Control Purposes

Uranium is the most common element in the nuclear fuel cycle. Different techniques have been used for analyzing the isotopic composition of uranium. Precise determination of uranium isotopic ratios for an efficient control of nuclear material was carried out through the modification of the used chromatographic method of uranium. Alpha spectrometry was utilized to identify different types of natural, depleted and enriched samples for safeguard purposes. Uranium element was extracted from other interfering radionuclides, purified, electrodeposited on a stainless-steel disc, and measured using alpha-spectrometer, then isotopic ratios were calculated. For comparison purposes, the samples were also measured using a hyper pure germanium (HPGe) spectrometer and the uranium isotopic ratios were obtained. The results obtained by both techniques were in agreement within difference ranged from -8.7 to 12%. It was concluded that alpha spectrometric measurements of uranium isotopes preceded by efficient radiochemical separation using extraction chromatography is a fast and reliable technique for safeguard purposes.

CONTENT OF URANIUM ISOTOPES IN THE GROUNDWATER SUPPLIES USED FOR POPULATION OF LENINGRAD REGION AND ST-PETERSBURG

The aim of the study was to obtain 234U and 238U specific activity in the water of groundwater supplies of Leningrad region and St-Petersburg and to estimate the possibility of their using from the point of view of radiation and chemical toxicity of the main dose-forming uranium isotopes usually containing in the underground waters. The study was focused on the water of functioning and exploratory groundwater supplies concerning the safety of water consumption taken into account radiation and chemical index. Data on the levels of natural uranium isotopes specific activity in the sources under investigation was obtained using radiochemical analysis with the subsequent alpha-spectrometric measurement of the counting samples. 58 samples of natural groundwater were analyzed during the period from February of 2011 till the May of 2017. The volume of the native water samples was from 10 l to 30 l, measuring time for each counting sample was 6 – 12 hours, which allowed measuring the radionuclides specific activity value at the level of 0.0002 Bq/kg. The values of 238U specific activity varied within 0.0002 Bq/kg – 0.06 Bq/kg, the average value was 0.007 Bq/kg. The values of 234U specific activity varied within 0.0006 Bq/kg – 0.111 Bq/kg, the average value was 0.013 Bq/kg. The average value of the specific activities ratio 234U/238U was 2.12 and the range of this value was 1.00 – 8.00. The results of carried out investigations demonstrates that the specific activity values of uranium isotopes could differ more then by an order of magnitude even in the borders of same aquifer of a small settlement. 238U specific activity value does not exceed 0.02 Bq/kg and 234U specific activity value does not exceed 0.04 Bq/kg for the vast majority of analyzed sample. The value of the ratio 234U/238U was 1.00 – 4.00 for 98.3% of analyzed sample. It is possible to conclude with a high probability that the water from the groundwater supplies of Leningrad region and St-Petersburg is safe for consumption by population concerning 234U and 238U content as from the point of view of radiological factor, so from the point of view of chemical toxicity.

Evaluation of several electrolyte mixture-cathode material combinations in electrodeposition of americium radioisotopes for alpha-spectrometric measurements

Three different types of electrolytes, subsequently modified and adjusted, in combination with three cathode materials used as source backings were analysed for electrodeposition of americium isotopes for alpha-spectrometric measurements. The obtained results are discussed in terms of electrodeposition yield and source quality (source homogeneity and spectral resolution, FWHM). The optimal conditions for source preparation are provided.

Daily variation of radon gas and its short-lived progeny concentration near ground level and estimation of aerosol residence time**Project supported by the Deanship of Scientific Research (DSR), King Abdulaziz University, Jeddah (Grant No. 291/965/1434).

Atmospheric concentrations of radon (222Rn) gas and its short-lived progenies 218Po, 214Pb, and 214Po were continuously monitored every four hours at the ground level in Jeddah city, Kingdom of Saudi Arabia. The measurements were performed three times every week, starting from November 2014 to October 2015. A method of electrostatic precipitation of positively charged 218Po and 214Po by a positive voltage was applied for determining 222Rn gas concentration. The short-lived 222Rn progeny concentration was determined by using a filter holder connected with the alpha-spectrometric technique. The meteorological parameters (relative air humidity, air temperature, and wind speed) were determined during the measurements of 222Rn and its progeny concentrations. 222Rn gas as well as its short-lived progeny concentration display a daily and seasonal variation with high values in the night and early morning hours as compared to low values at noon and in the afternoon. The observed monthly atmospheric concentrations showed a seasonal trend with the highest values in the autumn/winter season and the lowest values in the spring/summer season. Moreover, and in parallel with alpha-spectrometric measurements, a single filter-holder was used to collect air samples. The deposited activities of 214Pb and the long-lived 222Rn daughter 210Pb on the filter were measured with the gamma spectrometric technique. The measured activity concentrations of 214Pb by both techniques were found to be relatively equal largely. The highest mean seasonally activity concentrations of 210Pb were observed in the autumn/winter season while the lowest mean were observed in the spring/summer season. The mean residence time (MRT) of aerosol particles in the atmospheric air could be estimated from the activity ratios of 210Pb/214Pb.

Evaluation of sample pretreatment methods for analysis of polonium isotopes in herbal medicines

Herbal infusions like ayurvedic aristas are widely consumed by Indian population for good health. With increasing awareness about radiological assessment, an effort was made to assess the radioactivity concentration of naturally occurring radionuclides in herbal medicines. 210Po is an important alpha particle emitter contributing to internal dose to man from ingestion. Though 210Po can be spontaneously deposited on silver disk for alpha spectrometric measurements with less radiochemical step, great care has to be taken during the sample pretreatment step owing to the high volatility of polonium even at low temperatures. Aim of the study was to evaluate an appropriate sample pretreatment method for estimation of polonium in herbal medicines. 209Po was used for radiochemical yield calculation. Conventional open vessel wet ashing, physical evaporation, freeze-drying and microwave digestion in a Teflon vessel were examined. The recovery ranged between 9 and 79%. The lowest recovery was obtained for the samples that were processed by open vessel digestion without any volume reduction. The recoveries were comparable for those samples that were freeze dried and subjected to HNO3 + HClO4 + H2O2 + HF acid digestion and microwave digested samples. 210Po concentration in the samples ranged from 11.3 to 39.6 mBq/L.

Observation and modeling of 222Rn daughters in liquid nitrogen

The results of alpha spectrometric measurements of the activity of 222Rn daughters dissolved in liquefied nitrogen are presented. A direct detection method of ionized alpha-emitters from the 222Rn decay chain (214Po and 218Po) in a cryogenic liquid in the presence of an external electric field is shown. Properties of the radioactive ions are derived from a proposed model of ion production and transport in the cryogenic liquid. Ionic life-time of the ions was found to be on the order of 10s in liquid nitrogen (4.0 purity class). The presence of positive and negative ions was observed.

Optimization of low-background alpha spectrometers for analysis of thick samples

Results of alpha spectrometric measurements performed deep underground and above ground with and without active veto show that the underground measurement of thick samples is the most sensitive method due to significant reduction of the muon-induced background. In addition, the polonium diffusion requires for some samples an appropriate selection of an energy region in the registered spectrum. On the basis of computer simulations the best counting conditions are selected for a thick lead sample in order to optimize the detection limit.

A new method for the determination of low-level actinium-227 in geological samples

We developed a new method for the determination of 227Ac in geological samples. The method uses extraction chromatographic techniques and alpha-spectrometry and is applicable for a range of natural matrices. Here we report on the procedure and results of the analysis of water (fresh and seawater) and rock samples. Water samples were acidified and rock samples underwent total dissolution via acid leaching. A DGA (N,N,N′,N′-tetra-n-octyldiglycolamide) extraction chromatographic column was used for the separation of actinium. The actinium fraction was prepared for alpha spectrometric measurement via cerium fluoride micro-precipitation. Recoveries of actinium in water samples were 80 ± 8 % (number of analyses n = 14) and in rock samples 70 ± 12 % (n = 30). The minimum detectable activities (MDA) were 0.017–0.5 Bq kg−1 for both matrices. Rock sample 227Ac activities ranged from 0.17 to 8.3 Bq kg−1 and water sample activities ranged from below MDA values to 14 Bq kg−1of 227Ac. From the analysis of several standard rock and water samples with the method we found very good agreement between our results and certified values.

Evaluation of uncertainty and detection limits in 210Pb and 210Po measurement in water by alpha spectrometry using 210Po spontaneous deposition onto a silver disk

An easy and accurate method for the determination of 210Pb and 210Po in water using 210Po spontaneous deposition onto a silver disk is proposed and assessed for its detection capabilities according to the ISO Guide for the expression of uncertainty in measurement (GUM) and ISO Standard 11929-7 concerning the evaluation of the characteristic limits for ionizing radiation measurements. The method makes no assumption on the initial values of the activity concentrations of 210Pb, 210Bi and 210Po in the sample to be analyzed, and is based on the alpha spectrometric measurement of 210Po in two different aliquots: the first one measured five weeks after the sampling date to ensure radioactive equilibrium between 210Pb and 210Bi and the second after a sufficient time for the ingrowth of 210Po from 210Pb to be significant. As shown, for a recommended time interval of seven months between 210Po measurements, the applicability of the proposed method is limited to water samples with a 226Ra to 210Pb activity ratio CRa/CPb≤4, as usual in natural waters. Using sample and background counting times of 24h and 240h, respectively, the detection limit of the activity concentration of each radionuclide at the sampling time for a 1L sample typically varies between 0.7 and 16mBqL−1 for 210Pb in water samples with an initial activity of 210Po in the range 0–200mBqL−1, and between 0.6 and 8.5mBqL−1 for 210Po in water samples with an initial activity of 210Pb in the same range.

Sequential isotopic determination of plutonium, thorium, americium and uranium in the air filter and drinking water samples around the WIPP site

The simultaneous determination of actinides in air filter and water samples around the WIPP site have been demonstrated. The analytical method is based on the selective separation and purification by anion exchange and Eichrome-TEVA, TRU and DGA-resin followed by determination of actinides by alpha spectrometry. Counting sources for alpha spectrometric measurements were prepared by microcoprecipitation on neodymium fluoride (NdF3). Radiochemical yields were determined using 242Pu, 229Th, 243Am and 232U as tracers. The validation of the method is performed through the analysis of reference materials or participating in laboratory intercomparison programs. The plutonium concentrations in aerosols varied seasonally, being highest in spring and summer due to the spring-time enhanced wind-storm transportation of radioactive aerosols from the stratosphere to the troposphere. The 238Pu/239+240Pu activity ratio in the aerosol samples is typically close to that of global fallout from historic above-ground nuclear weapons testing. The results presented here indicate that the source of plutonium in the WIPP environment results mainly from global nuclear fallout and there is no evidence of increases in radiological contaminants in the region that could be attributed to releases from the WIPP.

Determination of plutonium from different sources in environmental samples using alpha-spectrometry and AMS

A reliable and sensitive method for the determination of plutonium in environmental samples by a combined use of alpha-spectrometry and accelerator mass spectrometry (AMS) is presented. Different environmental samples contaminated with plutonium from the Chernobyl accident and other sources were investigated using both methods. Plutonium was chemically separated using extraction chromatography. As a chemical yield tracer, 242Pu was applied for both AMS and alpha-spectrometry. After the alpha-spectrometric measurements, the samples were converted to targets suitable for the AMS measurements. AMS was especially chosen in addition to alpha-spectrometry, because it allows the determination of 240Pu/239Pu isotopic ratios as well as detecting the beta-emitting radionuclide 241Pu. Besides the generally used activity ratios of 238Pu/239,240Pu, there are now further optional isotopic ratios available using this method. By combining AMS with alpha-spectrometry, all relevant plutonium isotopes can be measured. Thereby a reliable distinction of different sources of plutonium in the environment is possible.

Preparation of alpha sources using magnetohydrodynamic electrodeposition for radionuclide metrology

Expanded use of nuclear fuel as an energy resource and terrorist threats to public safety clearly require the development of new state-of-the-art technologies and improvement of safety measures to minimize the exposure of people to radiation and the accidental release of radiation into the environment. The precision in radionuclide metrology is currently limited by the source quality rather than the detector performance. Electrodeposition is a commonly used technique to prepare massless radioactive sources. Unfortunately, the radioactive sources prepared by the conventional electrodeposition method produce poor resolution in alpha spectrometric measurements. Preparing radioactive sources with better resolution and higher yield in the alpha spectrometric range by integrating magnetohydrodynamic convection with the conventional electrodeposition technique was proposed and tested by preparing mixed alpha sources containing uranium isotopes ((238)U, (234)U), plutonium ((239)Pu), and americium ((241)Am) for alpha spectrometric determination. The effects of various parameters such as magnetic flux density, deposition current and time, and pH of the sample solution on the formed massless radioactive sources were also experimentally investigated.

Assessment of size-fractionated species of curium-244 via alpha spectrometry in groundwater

Curium was produced for experimental pro- grams for use as a heat source for isotopic electrical power generators and by 1968 approximately 5 kg had been pro- duced at the Savannah River Site (SRS). Size fractionated groundwater samples were collected near a disposal basin in F-Area at SRS in 1998 and in 2004. Separation of 244 Cm via extraction chromatographic methods was followed by alpha spectrometric measurement. In both years a trend of increasing Cm activities downstream of the seepage site was observed. Migration and immobilization resulting from base injection remediation between sampling dates explain large differences in 244 Cm concentration.

Traces of DU in samples of environmental bio-monitors (non-flowering plants, fungi) and soil from target sites of the Western Balkan region

This paper reports results of gamma and alpha spectrometric measurements for mosses, lichens, fungi and soil samples from areas in the Balkans targeted by depleted uranium (DU). Samples were collected in 2002 and 2003 in the vicinity of several villages, principally Han Pijesak (Bosnia and Herzegovina, hit by DU in 1995) and Bratoselce (South Serbia, hit by DU in 1999) and in lesser numbers from Gornja Stubla, Kosovo (which is identified as a high natural radon/thoron area) and Presevo close to the Kosovo border. In the course of gamma spectrometric measurements some results suggested samples with unusual high uranium contents which might be considered to be a signature for the presence of DU, although many samples had very high detection limits. Alpha spectrometric measurements directly proved the presence of DU for five samples, all from directly targeted places. These were samples of mosses, lichens and soil. For some samples homogeneity tests were applied which showed a rather even distribution of DU in these samples. No trace of DU was found in any sample from a dwelling.

Improved sample preparation method for environmental plutonium analysis by ICP-SFMS and alpha-spectrometry

A rapid and simple sample preparation method for plutonium determination in environmental samples by inductively coupled plasma sector field mass spectrometry (ICP-SFMS) and alpha-spectrometry is described. The developed procedure involves a selective CaF2 co-precipitation for preconcentration followed by extraction chromatographic separation. The proposed method effectively eliminates the possible interferences in mass spectrometric analysis and also removes interfering radionuclides that may disturb alpha-spectrometric measurement. For 239Pu, 240Pu and 241Pu limits of detection of 9.0 fg·g−1 (0.021 mBq), 1.7 fg·g−1 (0.014 mBq) and 3.1 fg·g−1 (11.9 mBq) were achieved by ICP-SFMS, respectively, and 0.02 mBq by alpha-spectrometry. Results of certified reference materials agreed well with the recommended values.

Determination of 226Ra in urine samples by alpha spectrometry

A radiation protection system to assess the internal contamination of workers during decontamination activities in an abounded fertilizer industry in the region of Attika, Greece, has been implemented. This system concerns, among other radionuclides, 226Ra. Because of the low 226Ra activities in urine, alpha spectrometry was used as the determination method after radiochemical separation. Radium was co precipitated with lead sulphate and purified using anion and cation exchange techniques. The source for the alpha spectrometric measurement was prepared by the electrodeposition of radium, from an aqueous/ethanol solution, onto stainless steel. The tracer used was 229Th. The chemical yield and the activity concentration were calculated via its daughter radionuclide 217At. Using the time-evolution formulas to calculate the 217At growth from its parent radionuclide 225Ra, a computer software was developed. This software was incorporated in a database, which automatically calculates and stores the results.

Lead fluxes, isotopic and concentration profiles in a peat deposit near a lead smelter (Příbram, Czech Republic)

The content and the isotopic composition of lead (Pb) were studied in a peat deposit on the ridge of the Brdy Hills, in the vicinity of the Príbram metallurgical works, in the Czech Republic. Quadrupole ICP MS was employed to determine the elemental composition and (206)Pb/(207)Pb and (208)Pb/(206)Pb isotope ratios. The individual layers were dated using alpha spectrometric measurement of the (210)Pb activity. The historical time period covered by the studied cores reached back to the 18th century. The Pb concentration in the studied profiles varied from 10 to 550 mg kg(-1). The (206)Pb/(207)Pb ratio varied in the range from 1.154 to 1.194 in the individual parts of the profile. The metallurgy of the Pb ores ((206)Pb/(207)Pb approximately 1.16), lithogenic Pb ((206)Pb/(207)Pb approximately 1.2), metallurgical processing of automobile batteries ((206)Pb/(207)Pb approximately 1.17) and the combustion of coal ((206)Pb/(207)Pb approximately 1.17-1.19) yield isotopic signatures that determine the isotope compositions of the individual profiles. Deposition rates between 15 mg m(-2) year(-1) at the beginning of the 19th century and 320 mg m(-2) year(-1) in the 1980s were determined in the dated profiles. The increased deposition rates determined on the dated profiles correspond to the increasing production of Pb ores in the Príbram mining area at the turn of the 19th and 20th centuries. The maximum for metallurgical production corresponds to the highest deposition rates recorded in 1960s and 1970s. The current deposition rate of 5-89 mg m(-2) year(-1) Pb is related to erosion of contaminated soils and waste dumps.