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.     

Radiochemical determination of210Po and210Pb in water

A method for²¹⁰Po and²¹⁰Pb determination in water samples is described. The nuclides are concentrated, in presence of added²⁰⁸Po and lead carrier, by evaporation. Then the polonium is plated electroless from the acidic solution on a copper planchet and measured by alpha spectrometry.²¹⁰Pb separation from the other isotopes is based on the solutility of PbSO₄ in citrate.²¹⁰Pb content is determined by measuring the activity of its daughter²¹⁰Bi. The critical steps in the isolation of lead have been examined and discussed.     

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.     

210Pb/210Po isotope generator

As a continuation of previous work (Kmak et al. in J Radioanal Nucl Chem 314:985–989, 2017), an isotope generator column based on the ²¹⁰Pb decay chain has been made to produce highly radiopure ²¹⁰Po. Two replicate studies were performed on AG 50Wx8 columns with an average yield of 90.4 ± 1.9%. ²¹⁰Pb breakthrough was seen at the 6 month elution for both generators.

     

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.     

Analysis of 210Pb and 210Po in Brazilian foods and diets

Radiochemical procedures for the analysis of ²¹⁰ Pb and ²¹⁰ Po in foods and diets are presented. Because of the low beta energy of ²¹⁰ Pb, its analysis was based on a separation of the daughter radionuclide ²¹⁰ Bi by precipitation of lead sulphate, ²¹⁰ Bi ingrowing and beta counting of this nuclide. ²¹⁰ Po analysis was based on wet dissolution of the sample, deposition onto silver disc and counting by alpha-spectrometry. Levels of these radionuclides in individual items and diets of selected university students were determined in order to evaluate the intakes of ²¹⁰ Pb and ²¹⁰ Po as well as the dose due to ingestion of foods and diets in São Paulo city.     

210Pb and210Po in tobacco-with a special focus on estimating the doses of210Po to man

Studies have been carried out on the solubility of Pu(III) oxalate by precipitation of Pu(III) oxalate from varying concentrations of HNO₃/HCl (0.5–2.0M) solutions and also by equilibrating freshly prepared Pu(III) oxalate with solutions containing varying concentrations of HNO₃/HCl, oxalic acid and ascorbic acid. Pu(III) solutions in HNO₃ and HCl media were prepared by reduction of Pu(IV) with ascorbic acid. 0.01–0.10M ascorbic acid concentration in the aqueous solution was maintained as holding reductant. The solubility of Pu(III) oxalate was found to be a minimum in 0.5M–1M HNO₃/HCl solutions containing 0.05M ascorbic acid and 0.2M excess oxalic acid in the supernatant.     

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.     

Determination of 210Pb, 210Bi and 210Po in natural drinking water

A new method for the radioanalytical determination of the ²²²Rn progenies ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Powill be presented, which has been improved for analyses of water samples fromdifferent regions in Austria. 1–2 liter samples were taken in polyethylenebottles prefilled with conc. HNO₃ to obtain 0.2M acidic solutions,thus avoiding adsorption effects. After adding 1.6 mg of inactive lead carrier,the water sample was evaporated to dryness, converted to the chloride formand dissolved in 1M HCl.     

The determination of low levels of polonium-210 in environmental materials

A method is presented for the determination of polonium-210 at very low levels in the presence of many different ions. Essentially quantitative recoveries were obtained in 60 min by deposition on to a silver plate in a special holder from 50 ml solution at 85–90° with sodium citrate present.     

Evaluation of measurement uncertainty in the determination of 210Pb and 210Po using beta counting and alpha spectrometry

 Measurement uncertainties in the determination of ²¹⁰Pb and ²¹⁰Po in Reference Material IAEA-300 (Baltic Sea Sediment) were evaluated. ²¹⁰Pb and ²¹⁰Po were separated from the matrix using an Sr resin column. The chemical yield of ²¹⁰Pb was determined gravimetrically in PbSO₄ form. Precipitation was followed by beta proportional counting after ²¹⁰Bi ingrowth. ²¹⁰Po was determined by alpha spectrometry after its spontaneous deposition on a Cu planchet. The major source of uncertainty was identified as the statistical counting uncertainty, which was also expected and is almost impossible to reduce without extension of the time required for an analysis. The expanded uncertainties were determined as 7.4% and 12.2% for ²¹⁰Pb and ²¹⁰Po, respectively. Received: 3 September 2002 Accepted: 3 December 2002 Acknowledgement This work was financially supported by Ministry of Education, Science and Sport, Republic of Slovenia (Project group PO-0106–0532). Presented at CERMM-3, Central European Reference Materials and Measurements Conference: The function of reference materials in the measurement process, May 30–June 1, 2002, Rogaška Slatina, Slovenia Correspondence to P. Vreˇcek     

Determination of environmental actinide nuclides and210Pb(210Po) by low-energy photon spectrometry with alpha-spectrometry

Low-energy photon spectrometry with -spectrometry was used to determine the environmental concentrations of low-level actinides and other nuclides, especially²¹⁰Pb and²¹⁰Po. The isotopic ratio of²⁴⁰Pu/²³⁹Pu was successfully determined by measuring L_x-ray/-ray counting ratio. A reliable method has been developed for the determination of extremely low-level²³⁷Np global fallout in environmental samples. The non-destructive determination by Ge-LEPS for natural²¹⁰Pb in various samples (tobacco leaves, commercially available tobacco, etc.) was also carried out with the determination of²¹⁰Po by -spectrometry using²⁰⁹Po as a yield tracer.     

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.     

A practical and accurate method for the determination of 234Th simultaneously with 210Po and 210Pb in seawater

A practical technique has been developed for the determinations of (234)Th simultaneously with (210)Po and (210)Pb in seawater samples, which greatly simplifies the on-board chemical procedures and enables an accurate correction of (234)Th ingrowth. A unique feature of this technique lies in the exact determination of co-precipitated (238)U following Fe(OH)(3) precipitation which leads to an exact correction of ingrown (234)Th between Fe(OH)(3) precipitation and U/Th separation. Such a correction eliminates several cumbersome on-board chemistry steps (such as Po plating, Fe(2+) oxidation, and 9 N HCl anion exchange) required in regular procedures to eliminate the (234)Th ingrowth. The total time required for on-board sample treatment (spike equilibration, Fe (OH)(3) co-precipitation and filtration) could be less than 10 h which significantly increases the sample processing efficiency and data throughput.     

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.

     

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.     

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 and210Po analysis in sediments and soils by microwave acid digestion

A microwave acid digestion method prior to the determination of²¹⁰Pb and²¹⁰Po in sediments and soils is described. It involves an acid (HNO₃, HCl, HF and H₃BO₃ mixture) digestion with microwave heating in closed vessels at high pressures. Analyses carried out for various reference materials showed that the results were statistically equal to certified values and reproducibility was also assured. The advantage of the microwave technique compared to the traditional leaching procedures is that the solid materials are completely dissolved and, therefore, ca. 100% efficiency is achieved in the extraction of²¹⁰Po and²¹⁰Pb, even though a fraction is associated to the silica net. Moreover, time of analysis is drastically reduced, as are the risks associated to vapour inhalation and material corrosion.     

Time-series observations of 210Po and 210Pb radioactivity in the western North Pacific

We carried out time-series observations of ²¹⁰Po and ²¹⁰Pb radioactivity in the western North Pacific Ocean. The sinking fluxes of particulate organic carbon (POC) in the mesopelagic zone were estimated from ²¹⁰Po radioactivity during several seasons in the subarctic and subtropical regions of the western North Pacific. The seasonal changes of POC fluxes at a depth of 400 m were larger in the subarctic region than in the subtropical region. The annual mean POC flux at a depth of 400 m was larger in the subarctic region (57 mgC m^?2 day^?1) than in the subtropical region (36 mgC m^?2 day^?1). The annual mean of the e-ratio (the ratio of POC flux to primary productivity) in the subarctic region (18 %) was about twice the e-ratio in the subtropical region (10 %). These results imply that the efficiency of the biological pump is larger in the subarctic region than in the subtropical region of the western North Pacific.     

210Po、210Bi和210Pb测试技术研究进展与现状

铀系核素210Po、210Bi和210Pb的测试在铀矿地质勘查与核废物安全处置研究、沉积年代学与同位素地球化学研究、大气环境学与辐射卫生学研究等诸多领域具有重要意义。重点总结了近些年来210Pb、210Bi和210Po三核素各种测试技术的研究进展与现状,评述了存在的主要问题及未来发展趋势。