An improved sensitive assay for polonium-210 by use of a background-rejecting extractive liquid-scintillation method

A procedure is described for the determination of polonium-210 in various types of materials, including ores, mill tailings, and environmental samples, by a combined solvent-extraction liquid-scintillation spectrometry method. Concentration of polonium-210 and separation from interfering elements (such as iron) are accomplished by extraction from a 7M phosphoric acid-0.01M hydrochloric acid solution with 0.20M trioctylphosphine oxide solution (together with a scintillator) in toluene. The polonium-210 is determined by counting the 5.3-MeV alpha-radiation with a photon/ electron-rejecting alpha liquid-scintillation spectrometer. Extraction coefficients of over 1000 for polonium ensure quantitative recovery, and no other alpha-emitters in the decay chains of uranium-238, uranium-235 and thorium-232 are extracted. The results for several samples show the relative standard deviation to be approximately 1.2%. A lower limit of detection of 0.0038 pCi is proposed, based on a counting time of 1000 min and an easily obtainable background of 0.01 cpm for the alpha peak.     

An example of situational radiological analysis: An incident with polonium-210

Data on the nuclear physical, chemical, and radiobiological characteristics of polonium-210 are generalized. The characteristics of the radionuclide intake by the human body, its transport, and deposition in different organs are considered. The formation of the α radiation dose has been analyzed using RBE = 3 for deterministic effects in terms of formal dosimetry of incorporated radionuclides. Radiological analysis of a case of polonium-210 poisoning in London has been performed. The activity of the radionuclide at which it is lethal upon a single peroral administration has been evaluated (0.012–0.36 GBq), and the formal possibility of detecting a carrier of polonium-210 on the basis of data on excreta and γ radiation measured using a whole-body counter (WBC).     

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.     

Improved technique for recovery and measurement of polonium-210 from environmental materials

Polonium-210 obtained in acidic solution by digestion of sediment or tissue samples is efficiently plated onto one side of a silver disc for measurement of α-activity. Optimum conditions for solutions obtained from environmental samples are pH 1.5–2 in the presence of citrate and ascorbic acid, with the solution at 80°C and the silver disc rotated at 100–150 radian s^?1. Observed recoveries using a polonium-208 tracer are 97.5 ± 2.5% for sediments and 99.3 ± 1.3% for tissues.     

Effects of digestion,chemical separation,and deposition on Po-210 quantitative analysis

The purpose of this work was to determine polonium losses from a variety of sample types (soil, cotton fiber, and air filter) due to digestion technique, chemical separation, and deposition method for alpha energy analysis. Results demonstrated that yields from a perchloric acid wet-ash (87 ± 5 %) were similar to that from a microwave digestion (100 ± 7 %), but both were greater than the dry-ash procedure (38 ± 5 %). The polonium was separated from an SRM soil using an AG1X8 ion exchange column and deposited on a Ag disk with a recovery of 83 ± 7 % of polonium-209 (Po-209). Deposition yields without chemical separation averaged 90 ± 5 % of Po-209. The polonium-210 content was successfully measured in the three matrix types and quantitated using alpha spectroscopy.     

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.     

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.

     

Rapid determination of 210Po in water samples

A new rapid method for the determination of ²¹⁰Po in water samples has been developed at the Savannah River National Laboratory (SRNL) that can be used for emergency response or routine water analyses. If a radiological dispersive device event or a radiological attack associated with drinking water supplies occurs, there will be an urgent need for rapid analyses of water samples, including drinking water, ground water and other water effluents. Current analytical methods for the assay of ²¹⁰Po in water samples have typically involved spontaneous auto-deposition of ²¹⁰Po onto silver or other metal disks followed by counting by alpha spectrometry. The auto-deposition times range from 90 min to 24 h or more, at times with yields that may be less than desirable. If sample interferences are present, decreased yields and degraded alpha spectrums can occur due to unpredictable thickening in the deposited layer. Separation methods have focused on the use of Sr Resin?, often in combination with ²¹⁰Pb analysis. A new rapid method for ²¹⁰Po in water samples has been developed at the SRNL that utilizes a rapid calcium phosphate co-precipitation method, separation using DGA Resin^® (N,N,N′,N′ tetraoctyldiglycolamide extractant-coated resin, Eichrom Technologies or Triskem-International), followed by rapid microprecipitation of ²¹⁰Po using bismuth phosphate for counting by alpha spectrometry. This new method can be performed quickly with excellent removal of interferences, high chemical yields and very good alpha peak resolution, eliminating any potential problems with the alpha source preparation for emergency or routine samples. A rapid sequential separation method to separate ²¹⁰Po and actinide isotopes was also developed. This new approach, rapid separation with DGA resin plus microprecipitation for alpha source preparation, is a significant advance in radiochemistry for the rapid determination of ²¹⁰Po.     

Sequential and rapid determination of Po-210, Bi-210 and Pb-210 in natural waters

A sequential and rapid separation method for the determination of radon daughter nuclides, Pb-210, Bi-210 and Po-210 has been developed for application to natural waters. Rapid separation is attained by the use of the same hydrochloric acid solution. After isolation of the three radionuclides from the sample by co-precipitation with added Fe³⁺, polonium isotopes are first spontaneously deposited onto a silver disc from a 0.5N hydrochloric acid solution. Next, bismuth isotopes are electrodeposited onto a platinum net cathode coupled with a platinum coil anode at 1.2 V. Finally, lead isotopes are electrodeposited onto a platinum net cathode at 1.8 V from the remaining solution by adding hydroxylamine hydrochloride as an anodic depolarizer. This method can be applied to meteorological precipitation samples where these three nuclides are separated within 10 hr after the sampling with chemical yields of more than 80% for Po-210 and Bi-210 and more than 70% for Pb-210. This method is applicable to other environmental water samples.     

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.     

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.     

226Ra, 210Pb, 210Bi and 210Po deposition and removal from surfaces and liquids

Deposition of ²²⁶Ra from water on nylon was investigated. Measurements performed for different pH and different radium concentrations in the water gave similar absolute activities deposited on the foil surface. Obtained results were used to estimate the amount of ²²⁶Ra plated-out on the nylon scintillator vessel in the solar neutrino experiment BOREXINO during filling of the detector. Another problem studied in the frame of BOREXINO was the removal of ²¹⁰Pb from its organic liquid scintillator by applying distillation and water extraction. After several tests had been performed for both methods it was found that after the water extraction the initial lead content in the scintillator sample was reduced only accordingly to the ratio of the volumes of the applied liquids (simple dilution). In contrast to this, distillation was very effective providing in the best case a ²¹⁰Pb reduction factor higher than 100. Removal efficiencies of the long-lived ²²²Rn daughters during etching from surfaces of standard and high purity germanium were investigated in the frame of the GERDA experiment, which aims to search for neutrino-less double beta decay of ⁷⁶Ge. The standard etching procedure of Canberra used during production of high purity n-type germanium diodes was applied to germanium discs, which had been exposed earlier to a strong ²²²Rn source for its progenies deposition. In contrast to copper and stainless steel, ²¹⁰Pb, ²¹⁰Bi and ²¹⁰Po was removed from germanium very efficiently. An evidence of a reverse process was also observed—the isotopes were transferred from the etchant to the clean germanium surface.     

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.

     

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.     

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.     

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.     

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.     

Determination of 210Po and uranium in high salinity water samples

A method for the determination of uranium and ²¹⁰Po in high salinity water samples has been elaborated. Both radionuclides are preconcentrated from 0.5 dm³ saline media by co-precipitation with hydrated manganese dioxide, followed by dissolution of the precipitate in 200 mL of 1 M HCl. Uranium isotopes ²³⁵U and ²³⁸U can be directly determined by ICP MS method with a detection limit of 0.01 ppb for ²³⁸U. Prior to a selective determination of ²¹⁰Po, the majority of other naturally occurring α-emitting radionuclides (uranium, thorium and protactinium) can be stripped from this solution by their extraction with a 50% solution of HDEHP in toluene. Finally, ²¹⁰Po is simply separated by direct transfer to an extractive scintillator containing 5% of trioctylphosphine oxide in Ultima Gold F cocktail and determined by an α/β separation liquid scintillation technique with detection limit below 0.1 mBq/dm³.     

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.     

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