Quantification of measurement uncertainty in the sequential determination of <Superscript>210</Superscript>Pb and <Superscript>210</Superscript>Po by liquid scintillation counting and alpha-particle spectrometry

Methodologies for the quantification of measurement uncertainties associated with the determination of ²¹⁰Pb- and ²¹⁰Po-specific activities by liquid scintillation counting (LSC) and alpha-particle spectrometry are presented, and are demonstrated using the soil reference material IAEA-326. Major contributors to the combined uncertainty associated with the measurement result of ²¹⁰Pb were the uncertainties of net count rates in the ²¹⁰Pb energy region of the sample spectrum and in the ²¹⁰Bi energy region of the blank spectrum. The predominant sources of uncertainty in the measurement of ²¹⁰Po were the uncertainties of net count rates in the regions of interest of ²⁰⁹Po and ²¹⁰Po. The relative standard uncertainty of ²¹⁰Po exponentially increases with the time interval between the sampling date and the separation date of Po, and this effect is strongly dependent on the ²¹⁰Po/²¹⁰Pb activity ratio. When the specific activity of ²¹⁰Pb is much higher than that of ²¹⁰Po in the sample, the relative standard uncertainty of the ²¹⁰Po determination increases significantly within a short time interval between the sampling date (or reference date) and the separation date of Po in samples.     

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.     

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.     

The fractionation and determination procedures for the speciation of Pb and Po in soil samples

A method for speciation and determination of ²¹⁰Pb and ²¹⁰Po in soil samples was developed. The speciation was carried out by fractionating the soil samples into five fractions which are water soluble or exchangeable, bound to carbonates, bound to Fe-Mn oxides, bound to organic matter and bound to residue. After mineralisation, 10% solution of each fraction was used to spontaneously deposit polonium on a silver disk at 85-90 °C and pH 1.5, and ²¹⁰Po was measured by α-spectrometry; the remain solution was used to separate lead by anion-exchange resin and purified by precipitation as PbS and PbSO₄, and ²¹⁰Pb was determined by a low background β-counter. The IAEA-327 reference material (soil) was studied for ²¹⁰Pb and ²¹⁰Po speciation. The results show that: (1) the average yields are 88.7 ± 6.4% for ²¹⁰Pb and 93.8 ± 8.2% for ²¹⁰Po; (2) if compared to the total ²¹⁰Pb activity in the sample, ²¹⁰Pb fractions are 0.95% in exchangeable form, 10.6% bound to carbonates, 14.3% bound to Fe-Mn oxides, 7.0% bound to organic matter and 67.2% bound to residue or acid soluble, and the corresponding values for ²¹⁰Po are 0.17%, 0.97%, 21.0%, 0.47% and 77.4%, respectively; and (3) the obtained ²¹⁰Pb concentration is in good agreement with the recommended value given by the IAEA.     

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.

     

Analytical methods to determine Po and Pb in marine samples

This paper describes the methods of sampling, preconcentration, chemical separation and final count of ²¹⁰Po and ²¹⁰Pb present in different marine matrices to determine their background levels in a marine ecosystem. Complex, time consuming and selective radioanalytical methods have been used to prepare final clear sources for alpha spectrometry and beta count; in fact, gamma spectrometry, a method direct and non destructive, cannot be taken into account because the ²¹⁰Pb activity is very low which does not allow to carry out sufficiently accurate measurements and ²¹⁰Po is not a gamma emitter but it emits only alpha particle at 5.40 MeV. The results of ²¹⁰Po and ²¹⁰Pb activity concentrations obtained in different marine samples collected in the first two campaigns are still very few to discuss about the ²¹⁰Po and ²¹⁰Pb behavior in marine environment.     

Marine Sediments and Snow from Ross Sea Region (Antarctica) Dating by 210Pb Method

Abstract

²¹⁰Pb is widely used to determine accumulation rates in order to obtain a time scale in environmental samples. The most accurate method uses the determination of ²¹⁰Pb via its grand-daughter ²¹⁰Po by alpha spectrometry. Unfortunately this method requires a complex wet-chemistry procedure to achieve the separation of ²¹⁰Po from its matrix. In this work a simplified procedure for the chemical separation of ²¹⁰Po is proposed and applied to three marine sediment cores and a 10 m snow core collected in Antarctica. The calculated sedimentation rates for marine sediments range from 0.053 to 0.071 cm y^?1. The mean annual accumulation rate for the snow is 16.6 cm y^?1 w.e. A comparison with literature data in the same region is given.     

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.

     

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.     

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.     

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.     

Distribution of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb in riverine environs of coastal Karnataka

The concentrations of ²¹⁰Po and ²¹⁰Pb have been measured in soil, sediment and rock samples collected from major rivers of coastal Karnataka, viz. Kali, Sharavathi and Netravathi. The activity of ²¹⁰Po and ²¹⁰Pb in the samples were separated by radiochemical methods and the activity was counted using ZnS(Ag) alpha-counter. The activity ratio of ²¹⁰Po and ²¹⁰Pb and the dependence of organic matter content on the activity of these radionuclides were studied.     

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.     

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.     

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.

     

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.     

Determination of 210Po in Reagent Samples by Alpha-Ray Spectrometry Using Extraction Chromatographic Resin

The determination of ²¹⁰Po in phosphoric acid reagent by alpha-ray spectrometry using extraction chromatographic resin is presented. The decontamination factors of interference elements were measured. It was observed that HCl, HNO₃, ascorbic acid, thioacetamide and Cu were free from ²¹⁰Po but Pb contain small amounts of ²¹⁰Po. ²¹⁰Po in phosphoric acid samples was ranged from <8 to 2.4 Bq/l. The detection limit of ²¹⁰Po in 50 ml of phosphoric acid is 8 mBq/l with a counting time of 1 day undercounting efficiency of 30%.     

Optimization of Pb determination via spontaneous deposition of Po on a silver disk

The accuracy of ²¹⁰Pb determination via spontaneous deposition of ²¹⁰Po on a silver disk and alpha spectrometric measurement was examined. The study focused on the storage conditions of the polonium-containing solutions, the tracer used in polonium analysis and the effect of storage time and acid concentration on ²¹⁰Po deposition. The intermediate precision and repeatability associated with the improved ²¹⁰Pb analysis of fresh groundwater samples was 5 and 14%, respectively. These improved values were achieved by using glass bottles as storage containers for the solution remaining from the first ²¹⁰Po deposition, by rinsing the sample container with concentrated hydrochloric acid after storage and by using different isotopes of polonium as the yield determinant tracer in the first and the second deposition. Less polonium adsorption onto the storage container walls occurred with HCl than with HNO₃. The overall uncertainty in ²¹⁰Pb analysis was (11 ± 7)% at the 95% confidence level. The minimum detectable activity concentration was 0.1 mBq l⁻¹ calculated from blank samples and 0.05 mBq l⁻¹ using the background counts of the alpha spectrometer.