Recycling of isotopically modified molybdenum from irradiated CerMet nuclear fuel: part 4—technetium separation from concentrated molybdate solution

Uranium-free molybdenum-based CerMet fuels can be applied for transmutation of minor actinides in GEN IV reactors or ADS. In a reprocessing concept designed in the first paper in this mini-series (Mareš and John in J Radioanal Nucl Chem 320(1):227–233, 2019. https://doi.org/10.1007/s10967-019-06456-2) the residual radionuclidic impurities need to be separated from slightly alkaline (pH 9.1) highly concentrated ammonium molybdate solutions. Screening tests of technetium extraction onto three extraction chromatographic materials were performed in present study. Solid extractants based on Aliquat^® 336 turned out to be the most promising for Tc extraction from molybdenum solutions both from the point of view of the extraction kinetics and the practical extraction capacity. The overall results of this mini-series allowed to conclude that if the molybdenum recycling concept proposed is adopted, separation of the residual radionuclidic impurities should not represent a significant problem.

     

Distribution of 210Po and 210Pb radionuclides and their dependence on physico-chemical parameters of soil in Madikeri taluk,Coorg district,Karnataka, India

The paper deals with distribution of ²¹⁰Po and ²¹⁰Pb radionuclides in a vertical profile of illuviated soil, in Madikeri taluk of Coorg district, Karnataka, India. The activity concentration of ²¹⁰Po and ²¹⁰Pb radionuclides was determined using radioanalytical method and the dependence of these radionuclides on physico-chemical parameters of soil was also investigated through a statistical study. In all the layers of the soil in a vertical profile, the ²¹⁰Po nuclides were found to be in disequilibrium with ²¹⁰Pb. The frequency distribution of ²¹⁰Po and ²¹⁰Pb radionuclides was analysed using Kolgomorov–Smirnov test.

     

Levels of 210Po and 210Pb in cigars

²¹⁰Po and ²¹⁰Pb concentrations have been determined in 58 cigar brands manufactured in 11 countries. Cuban and American cigars showed the lowest ²¹⁰Po content. The mean levels of ²¹⁰Po in Brazilian, European and Dominican cigars were almost identical and somewhat lower than the levels observed for cigars from other Latin American countries. Cuban, American and European cigars contained low levels of ²¹⁰Pb. Cigars from the remaining countries contained twice as much ²¹⁰Pb. The mean ²¹⁰Po/²¹⁰Pb ratio showed an excess of polonium. In the case of a one cigar-a-day smoker, the calculated annual absorbed dose due to ²¹⁰Po is -16 mGy.     

Measurement of lead-210, bismuth-210, and polonium-210 in environmental samples

Mathematical equations governing the ratio of²¹⁰Bi/²¹⁰Pb and²¹⁰Po/²¹⁰Pb activities are used to explain the ingrowth of²¹⁰Bi and²¹⁰Po in environmental samples during post collection. Procedures are described for radiochemical separation of²¹⁰Pb,²¹⁰Bi, and²¹⁰Po in a state of radioactive disequilibrium and quantification by alpha- and beta-counting. Also, the special case is considered where²¹⁰Bi is in equilibrium with²¹⁰Pb, but both are in disequilibrium with²¹⁰Po. In this case, the activities of both²¹⁰Pb and²¹⁰Po are computed by measuring²¹⁰Po activity twice, using alpha-counting.     

210Pb and 210Po radionuclides in the urban air of Lodz, Poland

The concentration of two important radionuclides: ²¹⁰Pb and its decay product ²¹⁰Po in the urban air in the center of the Polish city of Lodz were measured during the winter and spring seasons of 2008–2009. Urban airborne particulate matter was collected using two methods: an Anderson 9-stage impactor, and a high-volume aerosol sampler type ASS500 working in the frames of the aerosol sampling network in Poland, established for radionuclide monitoring. Average concentrations for 10 months sampling period for ²¹⁰Pb and ²¹⁰Po were 0.556 and 0.067 mBq/m³, respectively. However remarkable fluctuations due to meteorological condition were observed: from 0.010 to 0.431 mBq/m³ for ²¹⁰Po and from 0.167 to 1.847 mBq/m³ for ²¹⁰Pb. The highest concentrations, almost 60% of the total activities, of both radionuclides were found in the first two fine aerosol fractions with particle diameters below 0.36 μm. The aerosol residence times calculated from the ²¹⁰Po/²¹⁰Pb ratio ranged from 7 to 120 days.     

210Pb and 210Po concentrations in the Venice lagoon ecosystem (Italy) and the potential radiological impact to the local public and environment

In order to evaluate the possible radiological impact to the local public and environment from a phosphogypsum stockpile, ²¹⁰Po and ²¹⁰Pb concentrations in river water, lagoon water, suspended matter, superficial sediment, algae and bivalves samples collected in Venice lagoon area have been investigated. The results show that the mean ²¹⁰Po and ²¹⁰Pb concentrations in river water are 1.42±0.36 mBq^.l^-1 and 1.46±0.39 mBq^.l^-1 with a mean ²¹⁰Po/²¹⁰Pb ratio of 0.98±0.17 and about 60% of them are associated with the particulate; ²¹⁰Po and ²¹⁰Pb contribution from the phosphogypsum stockpile to the river water is negligible. Higher ²¹⁰Po (2.61-5.67 mBq^.l^-1) and ²¹⁰Pb (1.31-3.62 mBq^.l^-1) concentrations in the lagoon waters have been observed if compared with the literature values. About 60% of ²¹⁰Po and ²¹⁰Pb are found in the soluble form with a mean ²¹⁰Po/²¹⁰Pb ratio of 1.79±1.47. ²¹⁰Po and ²¹⁰Pb concentrations in 28 out 37 sediment samples ranged from 26 to 45 Bq^.kg^-1 (dry weight), only 9 sediments with ²¹⁰Po and ²¹⁰Pb concentrations greater than 45 Bq^.kg^-1 are found and most of them are located 1-4 km near the phosphogypsum stockpile. The elevated ²¹⁰Po and ²¹⁰Pb concentrations in the sediments may be due to the contamination from the phosphogypsum stockpile. The mean ²¹⁰Po/²¹⁰Pb ratio (0.986±0.049) in the sediments shows that ²¹⁰Po and ²¹⁰Pb exist in nearly secular equilibrium. ²¹⁰Po and ²¹⁰Pb concentrations in algae vary with different species. The mean ²¹⁰Po and ²¹⁰Pb concentrations in Gracilaria compress and Ulva laetevirens which show a similar behavior, are 3.18±1.23 Bq^.kg^-1 and 2.42±1.26 Bq^.kg^-1 (fresh weight), respectively, with a mean ²¹⁰Po/²¹⁰Pb ratio of 1.45±0.34. The mean concentration factors with respect to the filtered water are 1096±424 for ²¹⁰Po and 1299±680 for ²¹⁰Pb. The mean ²¹⁰Po and ²¹⁰Pb concentrations in the soft part of Mytilus edulis are 23.2±9.7 Bq^.kg^-1 and 0.537±0.203 Bq^.kg^-1 (fresh weight), respectively, with a mean ²¹⁰Po/²¹⁰Pb ratio of 43.6±10.0. The mean concentration factors with respect to the filtered water are 8006±3351 for ²¹⁰Po and 290±109 for ²¹⁰Pb, showing a very high accumulation effect for ²¹⁰Po. The accumulation behaviors of Cerastoderma glaucum and Tapes philippinarum for ²¹⁰Po are similar to Mytilus edulis, but that for ²¹⁰Pb seems less effective, corresponding to a relatively higher ²¹⁰Po/²¹⁰Pb ratio. The estimated committed effective doses from ²¹⁰Po for the individual local public through ingestion of bivalves are in the range of 0.050-0.231 mSv^.y^-1.     

Measurements of210Pb and210Po in Japanese human hair

²¹⁰Pb and²¹⁰Po in human hair have been measured to serve as an aid in order to estimate the dietary intake and body burden of these radionuclides of Japanese. The²¹⁰Po concentrations found in 83 hair samples were ranging from 4.0 to 59.3 mBq/g with a mean (median) value of 18.2±12.2 (14.9) mBq/g as compared to the²¹⁰Pb concentrations from 0.7 to 6.5 mBq/g with a mean (median) value of 2.3±1.1 (2.0) mBq/g. The²¹⁰Po/²¹⁰Pb activity ratios (mean: 8.7±5.1, median: 7.1) were surprisingly higher compared with the available literature value of about 2. The high concentration of²¹⁰Po in human hair of Japanese may be due to the ingestion of animal protein mainly in the form of seafood.     

A modified method for the sequential determination of 210Po and 210Pb in Ca-rich material using liquid scintillation counting

This research describes methods for the sequential determination of ²¹⁰Pb and ²¹⁰Po activity concentrations in Ca-rich ash samples collected from oil shale-fired power plants in Estonia. The procedure involves digestion of Ca-rich ash samples in a microwave digestion system, radiochemical separation of ²¹⁰Pb and ²¹⁰Po and their measurements. All samples, blanks and standards were measured by liquid scintillation counting (Quantulus 1220). The method was tested using IAEA (International Atomic Energy Agency) RGU-1 and IAEA-444 reference materials. Spectral calibration/peak identification which included the optimization of α/β discrimination system (pulse shape analyser), and recovery have been made by ²⁰⁹Po and ²¹⁰Pb standard solutions.

     

Correction to: Effect of pH,ionic strength and humic substances on the adsorption of Uranium (VI) onto Na-rectorite

Journal of Radioanalytical and Nuclear Chemistry - Correction to: J Radioanal Nucl Chem (2011) 287:557–565     

Estimation of sedimentation rates using 210Pb and 210Po at the coastal water of Sabah, Malaysia

Sediment cores were obtained from Teluk Brunei, Sipitang, Teluk Kimanis, Kota Kinabalu and Kuala Penyu at the coastal water of Sabah and analyzed for ²¹⁰Pb and ²¹⁰Po to estimate the sedimentation rates. The calculated sedimentation rates of ²¹⁰Pb and ²¹⁰Po varied from 0.003 to 0.049 cm/y and 0.74 to 8.77 cm/y, respectively. The highest sedimentation rates were determined for ²¹⁰Pb and ²¹⁰Po at stations located at Sipitang (mean: 0.027 cm/y) and Teluk Kimanis (mean: 5.53 cm/y), respectively. The sedimentation rate estimated for ²¹⁰Pb is not fully reliable because the activity of ²²⁶Ra was higher than that of ²¹⁰Pb and bioturbation was active at the sampling stations.     

Trace elements, 210Po and 210Pb in a selection of berries on commercial sale in Italy

The occurrence of ²¹⁰Pb, ²¹⁰Po, trace elements was assessed in a selection of berries on commercial sale in Italy. Data confirmed that berries might serve as an important source of essential elements. The ²¹⁰Pb, ²¹⁰Po concentrations found were higher than the reference values reported by UNSCEAR for roots and fruits in the world. There is no risk whatsoever from the intake of toxic elements as Al, As, Cd, Pb, Ni, Hg in berriberries analyzed; it is necessary, however, continuously monitored the levels of these elements to protect consumers against potential adverse health effects especially when consumed in large quantities.

     

The radiation dose and distribution coefficient of 210Po and 210Pb concentrations in aquatic environs of major rivers of coastal Karnataka

The activity of ²¹⁰Po and ²¹⁰Pb was measured in different matrices of aquatic ecosystem of the major rivers of Coastal Karnataka viz, Kali, Sharavathi and Netravathi. The environmental samples such as surface water, suspended particulate matter and sediment have been subjected to analyses. The activity of these two radionuclides were determined by radiochemical separation of ²¹⁰Po and counting the activity using a ZnS(Ag) alpha counter. The activity ratio of ²¹⁰Po and ²¹⁰Pb and correlation between the activity of these radionuclides were studied. From the measured concentration of ²¹⁰Po and ²¹⁰Pb, the internal Committed Effective Dose to the population for the study area was calculated. The distribution coefficient K_d between water, suspended particulate matter and sediments have been calculated to understand the distribution and accumulation of these radionuclides in different matrices of the aquatic environment.

     

Reply to query related to “Study of uranium contamination of ground water in Punjab state in India using X-ray fluorescence technique”

The queries made by Rathore in the preceding Letter to Editor (J Radioanal Nucl Chem, 2013) regarding the “Studies of ground water contamination in Punjab state in India using X-ray fluorescence technique” by Alrakabi et al. (J Radioanal Nucl Chem 294:221–227, 2012. doi: 10.1007/s10967-011-1585-x), are responded. The points raised by Rathore are important in case of sensitive analytical techniques, where only a small fraction (~few hundred μL of water) of the water sample collected in the container is effectively used as analyte. The biasing due to chemical speciation and physical escape of element of interest becomes significant in such rapid techniques if the ionic species of interest in the analyte are not stabilised using suitable additives. In the reported study based on X-ray fluorescence technique, the analyte used for elemental analysis was obtained by drying about 500–1000 mL of water sample. Adequate precautions were taken to minimize possibility of element of interest to escape or adhere to the bottle surface or lost as residue. The onsite acidification of collected water sample to pH 1 with reagent-grade nitric acid for sample preservation is not a pre-requisite in the procedure followed. The contribution of particulate matter to the reported concentrations of uranium was estimated to be insignificant. Also, the query related to effect of co-precipitation of uranium with formation of CaF₂ is found to be inconsequential. The comment made by Rathore (J Radioanal Nucl Chem, 2013) stating that ‘proceeding further in the measurement of uranium is a waste of time and has no meaning and results and discussion have no meaning too’ is extraneous.     

Atmospheric deposition of 210Po and 210Pb in Malaysian waters during haze events

Biogenic burning as forest fire phenomena occurring from April to August each year in the Sumatra and Borneo islands are major sources of biogenic uranium–thorium decay series in marine systems. 30 samples were collected during the Ekspedisi Pelayaran Saintifik Perdana 2009 cruise (EPSP 2009 cruise) between 12th June and 1st August 2009 from the Straits of Malacca to the Sulu and Sulawesi Seas to study the effect of haze and the monsoon season on the deposition rate of ²¹⁰Po and ²¹⁰Pb in Malaysian waters. All samples were spiked with 1 ml of lead [Pb(NO₃)₂; 25 mg ml^?1] and 0.05 ml of Polonium-209 tracer (26.08 dpm ml^?1). ²¹⁰Po activity was determined by auto plating onto silver foil and counting using an alpha spectrometry system (Canberra model Alpha Analyst with a silicon-surface barrier detector). Lead that was collected via electrodeposition, formed lead sulphate (PbSO₄) precipitation. This precipitate was wrapped onto plastic discs and counted for ²¹⁰Pb beta activity using a gross alpha–beta counting system (Tennelec model LB-5100 low background gas-flowing anti-coincidence alpha/beta counter) after 1 month to allow bismuth ingrowths. The range of ²¹⁰Po activities varied between 51.08 ± 15.1 and 742.08 ± 220.34 Bq/kg, whereas the activity of ²¹⁰Pb ranged from 31.10 ± 4.20 to 880.23 ± 123.86 Bq/kg and ²¹⁰Po/²¹⁰Pb ratio value varied between sampling stations from 0.19 to 13.77. The contents of ²¹⁰Po were also statistically positively correlated with the amount of total suspended particulate especially those recorded during heavy haze period events.     

Measurements of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb in total diet samples: Estimate of dietary intakes of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb for Japanese

To estimate the dietary intakes of ²¹⁰Pb and ²¹⁰Po for the Japanese adults and their annual effective doses, ²¹⁰Pb and ²¹⁰Po were measured for 240 daily diet samples collected at two locations of Ishikawa Prefecture in Japan over three years by duplicate portion studies. No appreciable differences in intake rates of ²¹⁰Pb and ²¹⁰Po and their ²¹⁰Po/²¹⁰Pb ratios were seen among the years in each district, and between the two districts. The intake rates evaluated using 240 diet samples were 0.20 Bq/d/p for ²¹⁰Pb and 0.61 Bq/d/p for ²¹⁰Po as a median, respectively. Annual effective doses of ²¹⁰Pb and ²¹⁰Po for Japanese adults were estimated to be 0.050 and 0.053 mSv/y, respectively.     

Polonium-210 and lead-210 in marine organisms: Intake levels for Japanese

The concentrations of²¹⁰Po and²¹⁰Pb were determined in about 30 species of marine organisms collected mainly from the north-easterm region of Japan to know the levels and distributions of these radionuclides and to estimate their intake levels from marine foods.²¹⁰Po and²¹⁰Pb showed a wide range of concentration in species: 0.6–26 and 0.04–0.54 Bq/kg (wet wt) in fishes, 0.5–220 and 0.2–43 Bq/kg (wet wt) in molluscs, echinoderms and chordatas, and 2.8–4.3 and 0.4–1.3 Bq/kg (wet wt) in algae, respectively. Higher accumulation of²¹⁰Po relative to²¹⁰Pb was found in all of the samples analyzed. The intake levels of²¹⁰Po and²¹⁰Pb by marine foods consumption were roughly estimated to be 0.48–0.69 and 0.022–0.042 Bq/d per person, respectively, on the basis of the statistical data on the consumption of seafood and/or production rates of marine foods.     

Determination of 210Pb and 210Po in mineral and biological environmental samples

The paper deals with the determination of ²¹⁰ Pb and ²¹⁰ Po in mineral and biological environmental samples. ²¹⁰ Pb and ²¹⁰ Po were preconcentrated from filtered water samples by coprecipitation with iron(III) hydroxide at pH 9-10 using ammonia solution and the precipitate was dissolved with HCl and mineralized with H2O2. ²¹⁰ Pb and ²¹⁰ Po in soil or sediment, algae and mussel samples were sequentially leached out at 250 °C with HNO₃ +HF, HClO₄ and HCl. About 10-20% of the leaching solution was used for ²¹⁰ Po determination which was carried out at 85-90 °C for 4 hours by suspending a silver disk in a HCl solution of pH 1.5 and containing some hydroxylamine hydrochloride and sodium citrate. No preliminary separation was required and essentially quantitative recoveries were obtained by using standard ²⁰⁹ Po tracer. The remains of the leaching solution were used for the determination of ²¹⁰ Pb which was first separated by a BIO-RAD-AG 1-X4 resin column, then purified by using Na2S to precipitate as PbS and finally precipitated as PbSO₄ for source preparation. Starting from 3 g sediment (30 liter water), the lower limits of detection of the method were 0.73 Bq.kg^-1 (0.078 mBq.l^-1 ) for ²¹⁰ Pb and 0.25 Bq.kg^-1 (0.016 mBq.l^-1 ) for ²¹⁰ Po. The procedure has been checked with two certified samples supplied by the International Atomic Energy Agency (IAEA) and reliable results were obtained. Most of the analyzed samples were sediments, showing average yields of 84.2±5.2% for ²¹⁰ Pb and 96.4±4.1% for ²¹⁰ Po.     

Presence and forms of210Pb,210Bi and210Po in ground level aerosols

A scheme of fractionation of²¹⁰Pb,²¹⁰Bi,²¹⁰Po forms present in air aerosols based on the combination of methods of radiochemical analysis and radiometric deteemination with leaching by different agents has been developed. The ratio between the²¹⁰Pb,²¹⁰Bi,²¹⁰Po present in the aerosol samples was determined experimentally. Carbonate of²¹⁰Pb, and²¹⁰Po and²¹⁰Bi forms connected with oxides prevai in the aerosol component of atmospheric air.     

Activity concentration of polonium-210 and lead-210 in tobacco products and annual committed effective dose to tobacco users in Tiruchirappalli District (Tamil Nadu,India)

The present study has carried out with an objective of determining the activity concentrations of two radionuclides namely polonium-210 (²¹⁰Po) and lead-210 (²¹⁰Pb) in smoke tobacco products (cigarette, bidi and cigar) and smokeless tobacco products (chewing tobacco and snuff) consumed in Tiruchirappalli District, Tamil Nadu (India) and their annual committed effective dose to tobacco consumers. The concentration of ²¹⁰Po was always higher than that of ²¹⁰Pb in all the analyzed tobacco products. It also revealed that 79% of Annual committed effective dose comes from ²¹⁰Po and about 21% from ²¹⁰Pb. Maximum concentration (13.2 mBq g^?1) of ²¹⁰Po recorded in cigarette and lowest concentration was observed in snuff (6.4 mBq g^?1). The highest mean committed effective dose of ²¹⁰Po and ²¹⁰Pb in various tobacco products were found in cigarette followed by bidi, cigar, chewing tobacco and snuff. The study revealed that the tobacco products available in Tiruchirappalli District contain a relatively lower concentration of radionuclides when compared to other regional studies. Since this kind of study in India is fragmentary, the present study has generated a base data for the first time for entire Tiruchirappalli District.

     

Determination of210Pb and210Po in human tissues of Japanese

To determine the levels of²¹⁰Pb and²¹⁰Po in human tissues of people in Japan, various tissue samples were obtained at autopsy from the cadavers of 22 oncologic cases, mainly in Niigata Prefecture in northern Japan, from 1986 to 1988.Wet ashing, followed by electrochemical deposition and alpha spectrometry were used to separate and determine the²¹⁰Pb and²¹⁰Po present. Among the tissues analyzed, the highest concentrations of²¹⁰Pb and²¹⁰Po were observed in bone (sternum), liver, and kidneys. The total body burden of²¹⁰Pb and²¹⁰Po was found to be approximately 427 pCi and 514 pCi, respectively. This estimated²¹⁰Po value did not differ significantly from values found in populations in the U.S.A. and European countries.