Measuring <Superscript>137</Superscript>Cs, <Superscript>40</Superscript>K and decay products of <Superscript>226</Superscript>Ra and <Superscript>232</Superscript>Th in samples of different nature by a multidetector spectrometer

A coincidence method for measuring ¹³⁷Cs, ⁴⁰K, ²²⁶Ra and ²³²Th decay products activity in soil, vegetation and fish samples, was applied to the six-crystal gamma-coincidence spectrometer PRIPYAT-2M. In this way, some problems appeared in simultaneous measurement of ¹³⁷Cs, ²²⁶Ra and ²³²Th by NaI(Tl) detectors and the PRIPYAT-2M spectrometer were solved. The obtained results were agreeable with the HPGe spectrometer ones.     

<Superscript>226</Superscript>Ra and <Superscript>228</Superscript>Ra determination in environmental samples by alpha-particle spectrometry

A complete methodology for ²²⁶Ra and ²²⁸Ra determination by alpha-particle spectrometry in environmental samples is being applied in our laboratory using ²²⁵Ra as an isotopic tracer. This methodology can be considered highly suitable for the determination of these nuclides when very low absolute limits of detection need to be achieved. The ²²⁶Ra determination can be performed at any time after the isolation of the radium isotopes from the analyzed samples while the ²²⁸Ra determination needs to be carried out at least six months later through the measurement of one of its grand-daughters. The method has been validated by its application to samples with known concentrations of these Ra nuclides, and by comparison with other radiometric methods.     

<Superscript>3</Superscript>H and <Superscript>90</Superscript>Sr in urine radiobioassay intercomparison results from the intercomparison studies program at Oak Ridge National Laboratory: statistical analysis of laboratory performance

The Intercomparison Studies Program (ISP) at the Oak Ridge National Laboratory (ORNL, Oak Ridge, TN USA) provides natural-matrix human urine quality-assurance/quality-control (QA/QC) samples to radiobioassay analysis laboratories. Samples are provided to these laboratories as “single-blind” or “double-blind” unknowns, spiked with radioactive-solution standards at “low” levels (e.g., 0.7–7 Bq g⁻¹ for ³H and 0.7–7 Bq kg⁻¹ for ⁹⁰Sr). Participants use the results as a tool for self-evaluation and a measure of performance. In this paper, sample preparation and the results of testing during the years 2001–2005 for ³H and ⁹⁰Sr are presented and discussed.     

Determination of <Superscript>93</Superscript>Zr in nuclear power plant wastes

A radioanalytical method (based on separation using UTEVA columns and ICP-MS measurement) has been used for determination of ⁹³Zr in 37 nuclear power plant samples. As ⁹³Nb might affect the detection of ⁹³Zr, Monte Carlo activation model was used to calculate the expected ⁹³Zr/^natZr mass ratio, which was compared to measured ones. It was found, that a decontamination factor of 10³ is sufficient to get a measurement uncertainty of less than 10%.     

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.     

Determination of <Superscript>151</Superscript>Sm and <Superscript>147</Superscript>Pm using liquid scintillation tracer methods

The long-lived rare earth isotopes ¹⁵¹Sm (90 years, β _max = 76.3 keV) and ¹⁴⁷Pm (2.62 years, β _max = 224.6 keV) are low-yield fission products that generally require lengthy separation procedures to isolate and count by their beta emissions. We will describe novel liquid scintillation counting techniques using radioactive tracers to determine radiochemical yields from an environmental matrix. The recovery of ¹⁵¹Sm is determined from the alpha decay (2.25 MeV) of ¹⁴⁷Sm in the natural Sm carrier and is in excellent agreement with the gravimetric recovery. The ¹⁴⁷Pm recovery is determined by the use of ¹⁴⁵Pm (17.7 years, EC) tracer, custom-produced at LANL using an isotopically enriched target of ¹⁴⁴Sm. We have determined the ¹⁴⁵Pm recovery both from the 37.4 keV k_α1 X-ray, and the electron-capture emissions by LSC. A comparison of these recovery methods is presented.     

Sequential separation of <Superscript>99</Superscript>Tc, <Superscript>94</Superscript>Nb, <Superscript>55</Superscript>Fe, <Superscript>90</Superscript>Sr and <Superscript>59/63</Superscript>Ni from radioactive wastes

A sequential separation procedure has been developed for the determination of ⁹⁹Tc, ⁹⁴Nb, ⁵⁵Fe, ⁹⁰Sr and ^59/63Ni in various radioactive wastes generated from nuclear power plants. Ion exchange and extraction chromatography were adopted for individual separation of the radionuclides. Precipitation was supplementarily utilized for both purification of the individual radionuclides and preparation of the radionuclide sources for use in a radioactivity measurement. The chromatographic separation behavior of the radionuclides both from the sample matrix metals and from one another was investigated using stable metals, Re (as a surrogate of ⁹⁹Tc), Nb, Fe, Sr and Ni. The validity of the procedure for reliability and applicability was evaluated by measuring the recovery of the metal carriers added to synthetic radioactive waste solutions. The recoveries by the chromatographic separation were in the range of 84.8 to 102.2% with 2s of less than 8.6%, the recoveries by the precipitation being in the range of 84.3 to 97.3% with 2s of less than 10.9%.     

Field measurement of the <Superscript>218</Superscript>Po, <Superscript>214</Superscript>Pb and <Superscript>214</Superscript>Bi concentrations in typical indoor and outdoor environments in Beijing

The activity concentrations of ²¹⁸Po, ²¹⁴Pb and ²¹⁴Bi [i.e. C(²¹⁸Po), C(²¹⁴Pb), and C(²¹⁴Bi)] and the calculated concentration ratios [i.e. 1:C(²¹⁴Pb)/C(²¹⁸Po):C(²¹⁴Bi)/C(²¹⁸Po)] are necessary for assessing radon and its progenies exposure. In this study, a measurement method of radon progenies concentrations with both high sensitivity and low uncertainty, was developed based on the Kerr method. The field measurement results of radon progeny concentrations and calculated concentration ratios in both typical indoor and outdoor environments in Beijing, China, were reported. The effects of air exchange rate on concentration ratios of radon progenies in indoor environments were discussed.     

Low level detection of <Superscript>135</Superscript>Cs and <Superscript>137</Superscript>Cs in environmental samples by ICP-MS

The measurement of fission product cesium isotopes ¹³⁵Cs and ¹³⁷Cs at low femtogram (fg) 10⁻¹⁵ levels in ground water by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) is reported. To eliminate the natural barium isobaric interference on the cesium isotopes, in-line chromatographic separation of the cesium from barium was performed followed by high sensitivity ICP-MS analysis. A high efficiency desolvating nebulizer system was employed to maximize ICP-MS sensitivity ~10 cps/fg. The three sigma detection limit for ¹³⁵Cs was 2 fg/mL (0.1 μBq/mL) and for ¹³⁷Cs 0.9 fg/mL (0.0027 Bq/mL) measured from the standard with analysis time of less than 30 min/sample. Cesium detection and 135/137 isotope ratio measurement at very low femtogram levels using this method in a spiked ground water matrix is also demonstrated.     

Disequilibrium of dissolved <Superscript>234</Superscript>U/<Superscript>238</Superscript>U and <Superscript>210</Superscript>Po/<Superscript>210</Superscript>Pb in Greek rivers

For the first time, a radiological study for the dissolved ²³⁸U, ²³⁴U, ²¹⁰Pb and ²¹⁰Po was held in major Greek rivers across the country. ²³⁴U/²³⁸U activity ratios are above one in all samples and ²¹⁰Po/²¹⁰Pb activity ratios are respectively below the unit indicating the disequilibrium in the samples. Quite satisfactory correlations were observed among ²³⁴U and ²³⁸U as well as among ²¹⁰Po and ²¹⁰Pb values. Uranium isotopes were separated by ion exchange and electroplated on stainless steel plates. ²¹⁰Po was spontaneously deposited on nickel plates, while ²¹⁰Pb was indirectly determined through the ingrowth of ²¹⁰Po. The sources were measured by a-spectrometry.     

<Superscript>234</Superscript>U/<Superscript>238</Superscript>U and <Superscript>235</Superscript>U/<Superscript>238</Superscript>U ratios in domestic water from the environs of Obuasi mine in Ghana

Activity concentrations of ²³⁸U, ²³⁵U and ²³⁴U were determined in different sources of drinking water at the Obuasi gold mines and its surrounding areas in Ghana. Water samples collected from the mines and its surrounding areas were analyzed using direct gamma-ray spectrometry and neutron activation analysis. The ²³⁴U/²³⁸U and ²³⁵U/²³⁸U ratios were calculated and the mean values range from 1.27 to 1.38 and from 0.044 to 0.045 respectively. The average ²³⁴U/²³⁸U ratio was from 1.27 for groundwater to 1.38 for treated water, demonstrating the lack of equilibrium. The average ²³⁵U/²³⁸U activity ratio is 0.045, indicating that only natural uranium was detected in the samples investigated.     

<Superscript>239</Superscript>Np as a tracer of <Superscript>237</Superscript>Np in effluent samples and low level nuclear waste

In this paper a technique to separate and measure both isotopes (²³⁷Np and ²³⁹Np) together is presented. A combined shape pulse discrimination liquid scintillation measurement with gamma-spectrometry, permits a precise measurement after the radiochemical separation. This technique was carried out by using an Eichrom chromatographic column (TEVA) as the first step of a more complete method, applied in the Nuclear Regulatory Authority, to separate actinides in nuclear waste and liquid effluents. The MCA is 0.08 Bq/l by alpha-spectrometry and 0.22 Bq/l (2σ) by liquid scintillation counting (LSC) for 93.7% of measurement efficiency and 98.4% of chemical recovery.     

Concentration of <Superscript>137</Superscript>Cs in seawater surrounding East Malaysia

Studies of ¹³⁷Cs distribution in East Malaysia were carried out as part of a marine coastal environment project. The results of measurements will serve as baseline data and background reference level for Malaysia coastline. Twenty-one locations were identified along the coastline of East Malaysia, and from each location water samples were collected at the surface of the seawater. Ten near-shore locations were also selected and seawater was collected at three different depths. Large volumes of seawater were collected and the co-precipitation technique was employed to concentrate cesium. A known amount of ¹³⁴Cs tracer was added as yield determinant, followed by addition of copper(II) nitrate salt and a solution of potassium hexacyanoferrate(II) trihydrate, to precipitate the total cesium. The precipitate slurry was oven dried at 60 °C for 1–2 days, finely ground and counted using gamma-ray spectrometry. The activity of ¹³⁷Cs was determined by measuring the peak area under the photopeak of the gamma-spectrum at 661 keV, which is equivalent to gamma-intensity corrected for detection efficiency, percentage of gamma-ray abundance of the radionuclide and recovery of ¹³⁴Cs tracer. There were no significant differences of ¹³⁷Cs activities both in surface and bottom water samples at 95% confidence level. The activity of ¹³⁷Cs (for all samples) was found to be in the range of 1.47 to 3.36 Bq/m³ and 1.69 to 3.32 Bq/m³ for Sabah and Sarawak, respectively.     

Determination of <Superscript>237</Superscript>Np, <Superscript>93</Superscript>Zr and other long-lived radionuclides in medium and low level radioactive waste samples

The majority of long-lived radionuclides produced in the nuclear fuel cycle can be regarded as “difficult-to-measure” nuclides, hence chemical separation is needed before the nuclear measurement of them. A combined radiochemical procedure that enables the simultaneous determination of some “difficult-to-measure” nuclides in medium and low level radioactive wastes has been developed in our laboratory. Recently, this method has been extended for determination of ²³⁷Np and ⁹³Zr. ²³⁷Np and ⁹³Zr are pre-concentrated by co-precipitation on iron(II) hydroxide and zirconium oxide, separated by extraction chromatography using UTEVA, and measured by inductively coupled plasma mass spectrometry (ICP-MS). As even traces of polyatomic ions and isotopes at m/z 237 or 93 cause considerable interferences during ICP-MS detection, a purification step by extraction chromatography was needed. Analyzing real samples (evaporation concentrates of a nuclear power plant) 66–99% and 31–99% chemical yields were achieved for Np and Zr, respectively.     

Preparation of calibration sources of <Superscript>88</Superscript>Kr and <Superscript>138</Superscript>Xe for HPGe detector

A method of efficiency calibration for the measurement of ⁸⁸Kr and ¹³⁸Xe by HPGe γ-spectrometer is proposed in the present paper. The question for the efficient calibration is, how to achieve homogeneous sources of ⁸⁸Kr-⁸⁸Rb and ¹³⁸Xe-¹³⁸Cs. The fission product gases were obtained by irradiating a precisely measured amount of U₃O₈ (90% ²³⁵U) filled in a quartz glass ampoule. Source cell was first filled up with stearic acid, and then the fission product gases were charged into it. Xenon and krypton are not adsorbed on stearic acid, therefore, homogeneous sources of ⁸⁸Kr-⁸⁸Rb and ¹³⁸Xe-¹³⁸Cs can be prepared. The results of the experiment demonstrate that the method is feasible and successful.     

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.     

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.     

ICP-MS analysis of plutonium activities and <Superscript>240</Superscript>Pu/<Superscript>239</Superscript>Pu ratio in alpha spectrometry planchet deposits

Plutonium isotopes were measured by alpha-spectrometry and ICP-MS in sediment samples from two European lakes: Blelham Tarn in U.K. and Stechlin lake in Germany. The ICP-MS measurements were made after alpha-spectrometry counting of the planchets. The planchets were prepared by traditional electrodeposition method after radiochemical extraction, separation and purification of the Pu fraction. A short radiochemical separation using plutonium selective resin, between the two spectrometry measures, is presented. The results show that these two complementary methods are in good agreement, the plutonium activity concentrations are the same. Alpha-spectrometry allows the ²³⁸Pu determination and ICP-MS individual measurement of ²³⁹Pu and ²⁴⁰Pu. ²³⁸Pu/^239+240Pu and ²⁴⁰Pu/²³⁹Pu ratios are calculated to determine the plutonium contamination source. With the results of these two techniques, it could be demonstrate that the plutonium is of global fallout origin.     

Measurement of the <Superscript>231</Superscript>Pa/<Superscript>235</Superscript>U ratio for the age determination of uranium materials

The paper describes the age (production date) determination of uranium reference materials using the ²³¹Pa/²³⁵U ratio. Direct addition of ²³⁷Np in secular equilibrium with its ²³³Pa daughter was chosen instead of the regular milking of ²³⁷Np to avoid possible loss of Pa. Sample preparation consists of a fast, one-step procedure. The developed method using ICP-MS for the measurement of ²³¹Pa is more precise than alpha spectrometry and is applicable for freshly produced low-enriched uranium materials. The measured ages are in good agreement with the reported production dates, thus the ²³¹Pa/²³⁵U chronometer can be applied for validation of ²³⁰Th/²³⁴U in nuclear forensics and safeguards.     

Preparation of <Superscript>26</Superscript>Al, <Superscript>59</Superscript>Ni, <Superscript>44</Superscript>Ti, <Superscript>53</Superscript>Mn and <Superscript>60</Superscript>Fe from a proton irradiated copper beam dump

The station for pions cancer therapy was operated at PSI from 1980 to 1992. After a cooling time of 12 years it’s made of copper beam dump was cut and samples were taken for analytical purposes. The sampling collected about 500 g of high active copper chips that can be used for separation of exotic radionuclides. The analyses by gamma spectrometry, LSC and AMS showed main nuclides present to be ⁶⁰Co, ⁵⁴Mn, ²²Na, ⁶⁵Zn, ²⁶Al, ⁵³Mn, ⁵⁹Ni, ⁶³Ni, ⁵⁵Fe and ⁶⁰Fe and ⁴⁴Ti with a daughter nuclide ⁴⁴Sc. In the frame of ERAWAST project a procedure combining selective precipitation and ion exchange for the separation of the rare radionuclides from the copper beam dump was developed. The proposed separation procedure is easy for remote controlled implementation in a hot cell. The ion exchange separation of Ni, Al, Mg, Ti and Fe was complete and high decontamination factors for copper and cobalt were achieved. Based on the developed procedure a remotely controlled system for separation of exotic radionuclides from the copper chips was set up. The full scale system was installed in a hot cell where high activity levels can be handled. In order to evaluate the reliability and functionality of the system extensive tests have been done. During the test period 13.86 g in total of the proton irradiated copper beam dump were processed for separation of ²⁶Al, ⁵⁹Ni, ⁵³Mn, ⁴⁴Ti and ⁶⁰Fe. The results showed that the system was operational and the radionuclide separation was selective with high chemical yield. The procedure manages as well the generated liquid wastes containing high level of ⁶⁰Co activity.