Ultra low level deep water <Superscript>137</Superscript>Cs activity in the South Pacific Ocean

We determined ¹³⁷Cs concentrations in deep water samples of the subtropical gyre in the South Pacific collected during the BEAGLE2003 cruise. This was done at an underground facility to achieve extremely low background γ-spectrometry, and we, therefore, obtained reliable values of ¹³⁷Cs activity in the deeper layers. ¹³⁷Cs activity in the layers between 2000 and 4500 m ranged from 7 ± 4 mBq m⁻³ to 25 ± 11 mBq m⁻³. The inventory of ¹³⁷Cs in the water column from 2000 m to the sea bottom was estimated to be 20 ± 8 Bq m⁻² to 94 ± 41 Bq m⁻² in this region.     

Soil-to-plant transfer factors of fallout <Superscript>137</Superscript>Cs and native <Superscript>133</Superscript>Cs in various crops collected in Japan

In order to compare the soil-to-plant transfer factors (TFs) of fallout ¹³⁷Cs and those of native stable ¹³³Cs, concentrations of these isotopes were determined in various crops and the associated soils collected throughout Japan. The results showed that TF-¹³⁷Cs was 11 times higher than TF-native ¹³³Cs for brown rice, while those values were almost the same for leafy vegetables. Possibly, fallout ¹³⁷Cs would be more mobile and more easily adsorbed by plants than native ¹³³Cs in the soil because a part of the ¹³³Cs is in a soil structure where it is hard to replace with ¹³⁷Cs. However, ¹³⁷Cs and native ¹³³Cs have reached an approximately isotopic equilibrium in the bioavailable fraction in the soils, therefore, the TF-native ¹³³Cs can be used for long-term transfer of ¹³⁷Cs in the environment.     

A novel electrochemical <Superscript>99</Superscript>Mo/<Superscript>99m</Superscript>Tc generator

A novel electrochemical process to avail clinical grade ^99mTc from (n,γ)⁹⁹Mo has been demonstrated. The electrochemical parameters were optimized to maximize the ^99mTc yield with minimal ⁹⁹Mo contamination. ⁹⁹Mo/^99mTc generators containing up to 29.6 GBq (800 mCi) ⁹⁹Mo were developed and their performance were extensively evaluated for 10 days without changing the operating conditions. Very high radioactive concentration of ^99mTcO₄ ⁻ of acceptable quality, commensurate with hospital radiopharmacy requirements could be availed from the system with >90% yield. The compatibility of the product for the formulation of ^99mTc labeled radiopharmaceuticals such as ^99mTc-DMSA and ^99mTc-EC was found to be satisfactory in terms of high labeling yields. The proposed route represents an important step for enhancing the scope of accessing clinical grade ^99mTc from low specific activity (n, γ)⁹⁹Mo.     

Determination of radionuclidic impurities in <Superscript>99m</Superscript>Tc eluate from <Superscript>99</Superscript>Mo/<Superscript>99m</Superscript>Tc generator for quality control

Technetium-99m is the principal radioisotope used in medical diagnostics; radionuclidic impurity is the major concern of its quality. This work presents a analytical method for sequential determination of all radionuclidic impurities listed in pharmacopoeia including gamma emitters, alpha emitters, ⁸⁹Sr and ⁹⁰Sr. Radioactive decay for removal of ^99mTc, ion exchange and extraction chromatography for removal of ⁹⁹Mo and ⁹⁹Tc are effective for separation of interferences. Gamma spectrometry, LSC with alpha/beta discrimination, and Cherenkov counting using LSC are sensitive methods for measurement of the impurity radionuclides. The detection limits of this method are well meet the requirement of the quality control according to the limitation of the pharmacopoeia.     

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.     

Measurement of <Superscript>99</Superscript>Tc in Savannah River Site high activity waste

Summary Waste cleanup efforts currently underway at the Savannah River Site have created a need to characterize ⁹⁹Tc in the various high activity waste matrices currently in Site inventories. The traditional method our laboratory used for analyzing ⁹⁹Tc in higher activity matrices was a solvent-solvent extraction method using Aliquat-336 in xylene. In an effort to eliminate the resulting generation of mixed wastes, a variety of different separation methodologies have been studied. Eichrom TEVA solid phase extractions using column technology have been employed in a case by case basis over the last several years. More recently, applications using Eichrom TEVA extraction discs and 3M Empore Tc extraction discs have also been explored.     

Distribution of <Superscript>137</Superscript>Cs around Kashiwazaki-Kariwa area

Cesium-137 distribution in several rivers, lakes and their sediments was investigated with HPGe detectors to elucidate the source of this isotope in some fresh waters from Kashiwazaki-Kariwa area, Niigata, Japan. It was suggested that there exists a place abundant in fallout radionuclides in the east side of a mountain which is located by the coast. Great westerly monsoon will contribute significantly to this phenomenon, which seems to be characteristic of mountains along the Sea of Japan.     

<Superscript>137</Superscript>Cs/<Superscript>137m</Superscript>Ba radioisotope generator based on 6-tungstocerate(IV) column matrix

Summary Barium-137m radioisotope generator of the chromatographic column elution mode based on loading 1.5 g 6-tungstocerate(IV) gel matrix with ~54 kBq of fission-produced ¹³⁷Cs is described. The elution performance of the generated ^137mBa radionuclide was investigated as a function of chemical composition of the eluent, flow rate, elution frequency, and age of the generator system. At comparable conditions, ^137mBa eluates with 0.9% NaCl-0.1M HCl eluent had higher elution yields and radionuclidic purity than with 0.1M NH₄Cl-0.1M HCl eluent. The generator has been repeatedly eluted for 311 days by passing 4810 ml of the saline eluent (10 ml × 481 elution operations) at a flow rate of 3.0 ml/min. Barium-137m eluates of high and reproducible elution yields, chemical and radionuclidic purities of (≥ 99.99%) were obtained.     

Constrains in gamma spectrometry analysis of fallout <Superscript>137</Superscript>Cs in coastal marine environment of Arabian sea in India

In this study, an accurate faster gamma spectrometry method for measuring the low level activity concentrations of ¹³⁷Cs using in situ pre-concentration technique on copper ferrocyanide cartridge was standardized. Due to unavailability of reference standard in the copper ferrocyanide matrix, efficiency calibration curves were plotted using RGU and RGTh reference standards. To harmonize the difference in density of standard and sample the required density correction factors for photo peak efficiency were generated. The in situ pre-concentration technique followed by gamma-ray spectrometry was applied for activity determination in surface seawater from eight locations in the coastal marine environment of Arabian Sea. The mean activity concentration of ¹³⁷Cs ranged between 0.71 and 0.91 Bq/m³. Higher activity concentrations were observed at location with latitude, longitude of 21.6°N, 69.57°E as compared to concentration observed at location with latitude, longitude 16.98°N, 73.25°E. The observed concentrations were found to be in range of data reported in Asia–Pacific Marine radioactive database (ASPARMARD). The results will fill up the gaps in the existing database. The generated data will be useful for monitoring fresh input of anthropogenic radionuclide into coastal marine environment for post Fukushima environmental assessment.     

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.     

Combined determination of <Superscript>99</Superscript>Tc and <Superscript>108m</Superscript>Ag in L/ILW liquid wastes

The low- and intermediate-activity level liquid wastes produced by the Paks Nuclear Power Plant (NPP) contain routinely measureable gamma-emitting (e.g., ⁵⁴Mn, ⁶⁰Co, ^110mAg, and ¹³⁷Cs) as well as many so-called “difficult-to-measure” radionuclides. Despite of their low specific activity compared to the total, the reliable determination of these radionuclides is an important issue of nuclear waste management. The increasing amount of waste samples to be qualified yearly by our laboratory put a pressure on revising the existing procedure of ⁹⁹Tc separation applied. We have managed to halve the initial amount of the sample required to achieve the same level of detection of technetium. Furthermore, one of the new purifying steps introduced have proved to be able to separate ^108mAg (and ^110mAg) better than 99% keeping the ⁹⁹Tc content of the product almost intact. Means of separation of ⁹⁹Tc from ¹⁰⁶Ru and ^124+125Sb have also been successfully investigated. As intended, this new procedure has a major impact on the chemical reagent as well as the electricity requirement of the separation making it more cost-effective.     

Relationships among <Superscript>137</Superscript>Cs, <Superscript>133</Superscript>Cs,and K in plant uptake observed in Japanese agricultural fields

Plant uptake of radiocesium (¹³⁷Cs) was investigated in consideration of the relationships with naturally existing ¹³³Cs and potassium (K). We first determined plant-unavailable fraction of ¹³⁷Cs in soil by batch sorption and sequential extraction methods with a radiotracer. Then, using the data obtained from the batch sorption and extraction methods, we clarified the relationships of plant-available and plant-unavailable fractions between ¹³⁷Cs, ¹³³Cs, and K in soil. Additionally, ¹³⁷Cs concentrations in crop were estimated using ¹³⁷Cs in soil and several factors, i.e. fixation ratio of ¹³⁷Cs in soil, cation exchange capacity, and K concentration in crop. The results implied that the fixation ratio of ¹³⁷Cs in soil was a very important key to understanding ¹³⁷Cs plant uptake.     

<Superscript>99</Superscript>Mo/<Superscript>99m</Superscript>Tc generators based on aluminum molybdate gel matrix prepared by nano method

A procedure for preparation of ⁹⁹Mo/^99mTc radioisotope generator based on low specific activity neutron activated ⁹⁹Mo was developed. Aluminum molybdate(VI)-⁹⁹Mo of high Mo(VI) content (~?364 mg/g Al⁹⁹Mo) was prepared by mixing low specific activity molybdate(VI)-⁹⁹Mo and aluminum mixture solution with isoamyl alcohol. Al⁹⁹Mo gel matrix was precipitated when the pH of the mixture solution was raised to ~?5 by addition of NaOH to the mixture. Radiometric measurements indicate the strong fixation of Molybdate(VI)-⁹⁹Mo species in the form of the sparingly insoluble Al⁹⁹Mo gel matrix. The prepared AlMo gel matrix was physiochemically characterized. Al⁹⁹Mo gel matrix was used as a base material for preparation of ⁹⁹Mo/^99mTc generator. The ^99mTc eluted from ⁹⁹Mo/^99mTc radioisotope generator was found to have relatively high elution yield (84?±?2.3%), radionuclidic (≥?99.99%), radiochemical (98.1?±?0.9%) and chemical purity.     

Determination of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr in the bottom sediments from the Barents Sea

The aim of this paper was to determine the extent of contamination by anthropogeneous radionuclides ¹³⁷Cs and ⁹⁰Sr in the bottom sediments from the Barents Sea based on the radioactive activity of the samples taken up in August 1991, among others, from the area close to New Land Island and Francis Joseph Archipelago. The results are based on the phenomenon of vertical migration, in the bottom sediments which is of significant importance from the natural environment point of view.     

Migration processes of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr in compartments of a lake ecosystem

Summary The dispersion of radioactive substances in the environment following nuclear weapon tests in atmosphere since 1954 and accidents to nuclear plants, like that in Chernobyl in 1986, have allowed us to study the migration processes of some radionuclides in complex ecosystems such as lakes are. In the present paper the behavior of ¹³⁷Cs and ⁹⁰Sr in different compartments of the Monterosi Lake (central Italy) was assessed. The ¹³⁷Cs concentration was measured in lake water as well as sediment, stream water, aquatic plant and fish samples. ⁹⁰Sr concentration in water and sediments was also determined. A total inventory of 4206±76 Bq ^. m^-2 and 958±79 Bq ^. m^-2 (on 27/6/01) has been found for ¹³⁷Cs and ⁹⁰Sr, respectively. The experimental data presented here allow to calibrate theoretical models predicting the temporal trend of radionuclide concentration in similar ecosystems. Moreover, information on cesium and strontium migration processes can be extended to other pollutants having similar environmental behavior.     

European measurement comparison of <Superscript>137</Superscript>Cs, <Superscript>40</Superscript>K and <Superscript>90</Superscript>Sr in milk powder

Recently, the Institute for Reference Materials and Measurements (IRMM) has assumed responsibility for organizing regular measurement comparisons among those laboratories which provide radioactivity monitoring data from their country to authorities of the European Commission (EC) under various EC legislation articles. The most recent exercise under this International Comparison Scheme for Radioactivity Environmental Monitoring (ICS-REM) in measuring the ¹³⁷Cs, ⁴⁰K and the ⁹⁰Sr activity concentration in milk powder is presented here. The complete cycle of the comparison is described, including the establishment of reference values traceable to SI units, the demonstration of the homogeneity of the distributed samples, the treatment and measurement of samples in the participating laboratories, and the evaluation of the results.     

Primary activity standardization of <Superscript>134</Superscript>Cs

Cesium-134 has been measured by means of a new coincidence counting system which is equipped with a liquid scintillation detector to count β particles and a NaI crystal to detect γ-rays which are emitted simultaneously. In order to validate this new technique, additional measurements were carried out with an established 4πβ–γ-coincidence counting system with a proportional counter in the β channel. The coincidence counting experiments were complemented with measurements in further liquid scintillation counters with two and three photomultiplier tubes. The counting efficiencies for these systems were determined using CIEMAT/NIST efficiency tracing and the triple-to-double coincidence ratio (TDCR) method, respectively.     

Evaluation of fresh and old eluate of <Superscript>99</Superscript>Mo/<Superscript>99m</Superscript>Tc generators used for labeling of different pharmaceutical kits

Summary Sixty ⁹⁹Mo/^99mTc wet column generators, loaded with two different ⁹⁹Mo activities, were analyzed in order to assess the quality of their eluates. Each elution was used for labeling of different radiopharmaceuticals, in order to evaluate whether “risky” elutions, namely those performed just after generator delivery and at 72 hours or more from the last elution, could be conveniently employed when fresh available radioactivity is not enough for the planned labeling or when shipping problems arise, or delay in delivery of a new generator occurs. Radiochemical quality control of all radiopharmaceuticals labeled with these elutions was performed. The elutions differed mainly in ⁹⁹Tc ground state (^99gTc) and amounts of oxidizing impurities. Radiolabeling procedures, however, were not affected, suggesting that these “risky” elutions might be appropriately used, in “emergency” conditions, for labeling radiopharmaceuticals although their radiochemical purity control is recommended prior to patient administration.     

Accumulation of <Superscript>137</Superscript>Cs and <Superscript>40</Superscript>K in aboveground organs of tropical woody fruit plants

Distribution of ⁴⁰K and ¹³⁷Cs in tissues of the Citrus aurantifolia was measured by gamma spectrometry. A simple theoretical model is also proposed to describe the temporal evolution of ⁴⁰K activity concentration in such tropical woody fruit species. This model exhibits close agreement with the ⁴⁰K experimental results, in the leaf growing and fruit ripening processes of lemon trees.     

Determination of the <Superscript>240</Superscript>Pu/<Superscript>239</Superscript>Pu atom ratio in global fallout at two locations in the Northern Hemisphere

Summary Extensive soil and sediment sampling was conducted along the Colorado Front Range and the plains east of the Front Range at locations believed to only be exposed to global fallout. The average ²⁴⁰Pu/²³⁹Pu atom ratio in the samples collected in Colorado was determined to be 0.165±0.008. A limited number of samples were collected at various locations in the Arctic at approximately 70° N latitude. Analyses of these samples predict that the ²⁴⁰Pu/²³⁹Pu atom ratio in environmental samples collected at 70° N latitude at locations only containing fallout is 0.183±0.009. These results provide data that help to precisely define the ²⁴⁰Pu/²³⁹Pu atom ratios representative of global fallout at the two locations studied.