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.     

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.     

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.     

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.     

A rapid method for the separation of 210 Po from 210 Pb by TIOA extraction

A rapid method for the separation of ²¹⁰ Po from ²¹⁰ Pb was developed utilizing extraction of triisooctylamine (TIOA)/xylenein HCl+H₂O₂ medium. Polonium in the form of PoCl ₆ ²– was extracted into TIOA phase and ²¹⁰Pb remains in the aqueous phase. Lead-²¹⁰ was determined by -countingof its granddaughter, ²¹⁰ Po ingrown from ²¹⁰ Pb forsome period of time. Distribution of ²¹⁰ Po and ²¹⁰Pb in TIOA and aqueous phases was investigated in various concentrations ofHCl media. Hydrogen peroxide was used to further decompose organic matterand to remove sulfur to prevent its deposition on the silver disc. The improvedprocedure resulted in a good chemical yield (80–95%) and a good á-resolution.     

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.     

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.     

The role of Cherenkov and liquid scintilation counting in evaluating the anion-exchange separation of210Pb−210Bi−210Po

Using as eluent a sequence of 3M HCl, 12M HCl, and 8M HNO₃, a mixture of²¹⁰Pb,²¹⁰Bi, and²¹⁰Po may be clearly separated on a column of Dowex 1×2−100 anion exchange resin. A Cherenkov count in H₂O and the variation in count rate with time confirm that the nuclides emerge in the order²¹⁰Pb→²¹⁰Bi→²¹⁰Po. If 12M HCl is replaced by 1.5M H₂SO₄/2.3 M Na₂SO₄, a clean separation also results, but recovery of²¹⁰Po becomes considerably more difficult. All three nuclides are readily detectable by liquid scintillation counting, with the efficiency for²¹⁰Pb in the 60–70% range. The Cherenkov aqueous counting efficiency for²¹⁰Bi is ∼14–15%.     

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     

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 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.     

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%.     

Improvements on the method for determining of <Superscript>210</Superscript>Pb and <Superscript>210</Superscript>Po in lead

An improved method is proposed to determine the content of ²¹⁰Pb in lead using ²¹⁰Po measured by alpha-ray spectrometry. This improved method, which is based on radiochemical separation by DDTC–toluene extraction, employs EDTA and citrate as masking reagents for the lead ions. To selectively extract polonium from an alkaline solution, the pH dependency was examined using a liquid scintillation counting method. And pH 9 was chosen as an extraction condition. Then ²¹⁰Po was electrodeposited on a stainless steel disk, and the chemical recovery was followed by ²⁰⁹Po tracer. The effectiveness of the new method was validated by the agreement with the analytical results from five samples as determined by gamma-ray spectrometry.     

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.     

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.     

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.     

Simultaneous determination of210Bi and210Po on pine needles by solvent extraction and liquid scintillation counting

A determination procedure has been developed for²¹⁰Bi and²¹⁰Po in environmental samples and was applied for pine needles. Bismuth-210 and²¹⁰Po separated from the parent nuclide²¹⁰Pb as BiOCl precipitate were extracted simultaneously by TOPO/toluene containing PPO and POPOP. The separation of²¹⁰Bi and²¹⁰Po from²¹⁰Pb was almost satisfactory. The activity of²¹⁰Bi+²¹⁰Po in the TOPO/toluene was measured periodically by liquid scintillation counting for about 20 days after separation. The time course of the decreasing pattern of the activity was determined by the initial activity ratio²¹⁰Po/²¹⁰Bi. The decreasing pattern of the activity was compared with theoretical patterns, and best estimates for²¹⁰Po and²¹⁰Bi were obtained by non-linear least-squares fitting. The activities of²¹⁰Bi and²¹⁰Po were determined for one-year and two-year old pine needles fro the same pine tree, and weathering half-time and deposition rate of these nuclides was discussed.     

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.     

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.