Distribution of fallout radionuclides through soil surface layer

The distribution of¹³⁷Cs through soil layers has been investigated by field sampling. The investigation deals with¹³⁷Cs concentration found after the Chernobyl accident. The relationship between important soil characteristics, total precipitation and cesium distribution are analyzed. Cesium is strongly sorbed in the top soil layer and its migration downward is limited. Measurements performed over a 3-year period revealed that approximately 20–38 per cent of total¹³⁷Cs is located in the upper soil layer.     

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.     

Improvement of <Superscript>137</Superscript>Cs analysis in small volume seawater samples using the Ogoya underground facility

¹³⁷Cs in seawater is one of the most powerful tracers of water motion. Large volumes of samples have been required for determination of ¹³⁷Cs in seawater. This paper describes improvement of separation and purification processes of ¹³⁷Cs in seawater, which includes purification of ¹³⁷Cs using hexachloroplatinic acid in addition to ammonium phosphomolybdate (AMP) precipitation. As a result, we succeeded the ¹³⁷Cs determination in seawater with a smaller sample volume of 10 liter by using ultra-low background gamma-spectrometry in the Ogoya underground facility. ¹³⁷Cs detection limit was about 0.1 mBq (counting time: 10⁶ s). This method is applied to determine ¹³⁷Cs in small samples of the South Pacific deep waters.     

A simple preparation of calibration curve standards of134Cs and137Cs by serial dilution of a standard reference material

Two sets of calibration standards for¹³⁴Cs and¹³⁷Cs were prepared by small serial dilution of a natural matrix standard reference material, IAEA-154 whey powder. The first set was intended to screen imported milk powders which were suspected to be contaminated with¹³⁴Cs and¹³⁷Cs. Therefore the concentration range of the calibration standards were about 40–400 Bq/kg. The precision of the preparation of the standard with about 7 Bq/kg of¹³⁴Cs and 39 Bq/kg of¹³⁷Cs at measurement time was 7.4% and 3.2%, respectively. The preparation of a similar standard by spiking the matrix with radioisotope solutions resulted in a poorer precision, about double that of the former technique. The other set of calibration standards was prepared to measure the environmental levels of¹³⁷Cs in commercial Venezuelan milk powders. Their concentration ranged from 3–10 Bq/kg of¹³⁷Cs. The accuracy of these calibration curves was checked by using IAEA-152 and A-14 milk powders. Their measured values were in good agreement with their certified values. Finally, it is shown that these preparation techniques by serial dilution of a standard reference material were simple, rapid, precise, accurate and cost-effective.This work was partly funded by a research contract PC-075 from the Consejo Nacional de Investigaciones Científicas y Tecnológicas (CONICIT).     

Depth profiles of long lived radionuclides in Chernobyl soils sampled around 10 years after the accident

Depth profiles of the long-lived radionuclides, ¹³⁷Cs, ⁹⁰Sr, Pu isotopes and ²⁴¹Am were examined in undisturbed sandy, peaty and Podsol soils in the Chernobyl 30 km exclusion zone sampled around 10 years after the accident. Two Podsol soils, which have different radioactive deposition characteristics, have also been examined. Activity ratios of ^239,240Pu/¹³⁷Cs, ⁹⁰Sr/¹³⁷Cs, and ²⁴¹Am/¹³⁷Cs in the 0-1 cm layer of the two Podsol soils differed very much. Speciation of the radionuclides by sequential selective extraction was examined in the soils. Depth profiles of the soils have been analyzed according to the speciation results and soil characteristics.     

Recovery of137Cs from acidic fission products solutions

A procedure for the isolation of¹³⁷Cs from acidic fission products solutions, based on the use of silica gel and zirconium phosphate ion exchangers, is presented. The¹³⁷Cs recovered by the ion-exchange process is converted to powder by coprecipitation of cesium with ammonium molybdophosphate.¹³⁷Cs pellets have been prepared by compression of¹³⁷Cs ammonium molybdophosphate powder using a hydraulic press. An important aspect of this procedure is that it does not require neutralization of the Purex waste.     

Study on the preparation of a137Cs/137mBa radionuclide generator

^137mBa has been applied successfully to dynamic studies for diagnosis in nuclear medicine for a long time. A variety of inorganic exchangers have been employed for the separation of^137mBa from its parent¹³⁷Cs. In the present study, cupric cobaltic ferrocyanide and amorphous zirconyl phosphate were synthesized and compared for use in a¹³⁷Cs/^137mBa generator. The results show that the former can adsorb¹³⁷Cs more efficiently and provide high elution yield of^137mBa with greater than 99.99% radionuclide purity. A new generator involving multimillicuries of^137mBa, in connection with a computerized detection system, has been constructed.     

Determination of Cs and Cs in environmental samples: A review

Radionuclides of caesium are environmentally important since they are formed as significant high yield fission products (¹³⁵Cs and ¹³⁷Cs) and activation products (¹³⁴Cs and ¹³⁶Cs) during nuclear fission. They originate from a range of nuclear activities such as weapons testing, nuclear reprocessing and nuclear fuel cycle discharges and nuclear accidents. Whilst ¹³⁷Cs, ¹³⁴Cs and ¹³⁶Cs are routinely measurable at high sensitivity by gamma spectrometry, routine detection of long-lived ¹³⁵Cs by radiometric methods is challenging. This measurement is, however, important given its significance in long-term nuclear waste storage and disposal. Furthermore, the ¹³⁵Cs/¹³⁷Cs ratio varies with reactor, weapon and fuel type, and accurate measurement of this ratio can therefore be used as a forensic tool in identifying the source(s) of nuclear contamination. The shorter-lived activation products ¹³⁴Cs and ¹³⁶Cs have a limited application but provide useful early information on fuel irradiation history and have importance in health physics.     

Soil-to-mushroom transfer of <Superscript>137</Superscript>Cs, <Superscript>40</Superscript>K,alkali–alkaline earth element and heavy metal in forest sites of Izmir,Turkey

The present work is devoted to an investigation on the soil to mushroom transfer parameters for ¹³⁷Cs and ⁴⁰K radionuclides, as well as for some stable elements and heavy metals. The results of transfer factors for ¹³⁷Cs and ⁴⁰K were within the range of 0.06–3.15 and 0.67–5.68, respectively and the most efficiently transferred radionuclide was ⁴⁰K. The TF values for ¹³⁷Cs typically conformed to a lognormal distribution, while for ⁴⁰K showed normal distribution. Statistically significant correlations between ¹³⁷Cs soil to mushroom transfer factors and agrochemical soil properties have been revealed. Although the concentration ratios varied within the species, the most efficiently transferred elements seems to have been K, followed by Rb, Zn, Cu, Cd, S, Cs and Hg.     

Removal of137Cs from an intermediate level liquid waste by using various ion-exchange media

An intermediate level liquid waste (ILLW or Category III waste) stream was treated for the removal of radioactive Cs in pilot scale experiments, using three different ion exchange media. Results indicated that the polyacrylic fibre coated with cupric ferric hexacyanoferrate (CuFeHCF-fibre composite) was the most efficient, followed by cupric hexacyanoferrate loaded ion exchange resin (CuHCF-resin) and mixed zeolites (AR-1, 4A and 13X in the ratio 6:1:1). The mixed zeolites column and the CuFeHCF-fibre column were used in series in order to get a high total decontamination factor (DF). Leaching studies on the CuFeHCF-fibre composite loaded with¹³⁷Cs, in demineralised (DM) water, tap water and ground water media indicated a release of about 19.3%, 25.5% and 41.3% of¹³⁷Cs, respectively, in a period of about 8 months. XPS studies with CuFeHCF-fibre composite indicated some chemical interaction between the CuFeHCF precipitate and the polyacrylic fibre. Some of the possible disposal options for the CuFeHCF-fibre composite have also been discussed.     

137Cs activity in surface water in the western North Pacific

Temporal and spatial variations of ¹³⁷Cs activity in surface waters in the western North Pacific are examined along the 165°E transect. ¹³⁷Cs in seawater of the western North Pacific has been introduced by global fallout originating from atmospheric nuclear weapons tests, which caused major fallout in the early 1960's. At this time ¹³⁷Cs activities in the surface waters in mid latitudes of the North Pacific were 10–20 Bq·m^-3. South of 30°N, ¹³⁷Cs activity decreased gradually towards the south. The surface ¹³⁷Cs activity was about 5 Bq·m^-3 in the Equatorial region. In the 1970's, the difference in ¹³⁷Cs activities in surface water between mid latitudes and the Equatorial region became smaller. The ¹³⁷Cs activity in surface water at 40°N – Equatorial region was almost constant at the level of 1.7–3.7 Bq·m^-3 in the late 1990's. In the Equatorial region, the ¹³⁷Cs activity in surface water showed no temporal change except for radioactive decay over these four decades. The surface ¹³⁷Cs level was 1.4–1.8 Bq·m^-3 in the north subarctic region around 50°N in the late 1990's. The lower ¹³⁷Cs activity may have been caused by deeper convection in this sea area and dilution by fresh water flux.     

Radionuclide variations in the air over Monaco

Radionuclides in aerosols and precipitation have been analyzed by IAEA-MEL in Monaco since 1987 and 1999, respectively, to identify their behavior in the atmosphere and delivery into the northwestern Mediterranean Sea. While the concentration of ⁷Be in aerosols has been affected by the stratospheric-tropospheric mixing and precipitation, the concentration of ¹³⁷Cs in aerosols has been influenced by a combination of local meteorological conditions and re-suspension of ¹³⁷Cs from soil. Higher concentrations of ⁷Be, ¹³⁷Cs, ^239,240Pu and ²⁴¹Am in precipitation occurred during spring and summer. The highest deposition rates of these radionuclides were observed in spring and autumn during periods of high precipitation. A good correlation was found between the amount of precipitation and depositional flux for ⁷Be, but not for ¹³⁷Cs, ^239,240Pu and ²⁴¹Am. This indicates that the wet process as well as the dry process seem to be important factors in determining the annual deposition for transuranic radionuclides and ¹³⁷Cs.     

Depth distribution of239,240Pu and137Cs in soils of South Korea

Depth distribution of^239,240Pu and¹³⁷Cs in the soils of South Korea have been studied. The average accumulated depositions were estimated roughly to be 54.8±32.1 Bq·m^–2 for^239,240Pu, 1.6±1.0 Bq· ·m^–2 for²³⁸Pu and 1982.8±929.1 Bq·m^–2 for¹³⁷Cs. The activity ratios of^239,240Pu/¹³⁷Cs in soils were found to be in the narrow range of 0.0153 to 0.0364 with a mean value of 0.0230±0.006. The concentrations of^239,240Pu and¹³⁷Cs in soils decrease exponentially with increasing the soil depth. A significant correlation was found between the concentration of^239,240Pu and that of¹³⁷Cs. The activity ratios of^239,240Pu/¹³⁷Cs tend to increase slightly with increasing soil depth.     

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.     

Fallout 137Cs in soils from North Western Libya

Fallout levels of ¹³⁷Cs in surface soil from North WesternLibya have been measured using gamma-ray spectrometry. The activity concentrationsof ¹³⁷Cs in soil ranged from 975 to 1720 mBq . kg ^—1 . The areal activity concentrations ranged from 1300 to 2250 mBq .m ^—2 , and were higly correlated with annual precipitation.The effective dose from external exposure to ¹³⁷Cs is found tobe 3 nSv . y ^—1 .     

Cesium-137 content in blood of Taiwan residents

Samples of blood from adults in good health in Taiwan have been analyzed for their¹³⁷Cs content by gross beta counting using a low background gas-flow counter. The level of¹³⁷Cs content in blood was 8.3+6.3x10^–3 pCi.ml^–1 for ages 24+7 y. The deposition of fission product¹³⁷Cs in Taiwan, which was monitored by water tray for fallout, was also studied since January 1979.     

137Cs transfer from forage to milk and its removal by clay treatment

Since April 29, 1986, the radioactive contamination resulting from the accident of the Chernobyl reactor has been measured in various kinds of matrixes, with particular regard to Northern Italy. Here we present the data obtained for¹³⁷Cs from several measurements effected on milk and dairy products over the period of one year. In particular, we have studied the transfer kinetics of¹³⁷Cs from forage to milk by feeding dairy cows with forage of known activity and we have evaluated the body Cs absorption by measuring the percentages of Cs eliminated with milk as well as with urine and feces. Further, the decay rate of¹³⁷Cs in milk has been assessed and the results of the kinetic, analysis are reported. We have also evaluated the efficacy of various clay materials in removing Cs from milk. Here we report the results of adsorption kinetics for the grey clay which resulted the most effective material.     

Separation of 134Cs and 133Ba radionuclides by calcium alginate beads

The uptake behavior of long-lived radionuclides such as ¹³⁴Cs (2.06 years), ¹³⁷Cs (30 years) or ¹³³Ba (10.54 years) on calcium alginate (CA) beads have been investigated. The CA beads are able to remove ¹³³Ba (92%) at pH 7 after 90 min of exposure from the binary mixture of two. The separation method of short-lived daughter ¹³⁷Ba (2.55 min) from its long-lived parent ¹³⁷Cs (30 years) using this CA beads have also been developed.     

Comparison of thermal ionization mass spectrometry and Multiple Collector Inductively Coupled Plasma Mass Spectrometry for cesium isotope ratio measurements

In the nuclear domain, precise and accurate isotopic composition determination of elements in spent nuclear fuels is mandatory to validate neutron calculation codes and for nuclear waste disposal. The present study presents the results obtained on Cs isotope ratio by mass spectrometric measurements. Natural cesium is monoisotopic (¹³³Cs) whereas cesium in spent fuels has 4 isotopes (¹³³Cs, ¹³⁴Cs, ¹³⁵Cs, and ¹³⁷Cs). As no standard reference material is available to evaluate the accuracy of Cs isotopic measurements, a comparison of cesium isotopic composition in spent nuclear fuels has been performed between Thermal Ionization Mass Spectrometry (TIMS) and a new method involving Multiple Collector Inductively Coupled Plasma Mass Spectrometry (MC-ICPMS) measurements. For TIMS measurements, isotopic fractionation has been evaluated by studying the behavior of cesium isotope ratios (¹³³Cs/¹³⁷Cs and ¹³⁵Cs/¹³⁷Cs) during the analyses. For MC-ICPMS measurements, the mass bias effects have been corrected with an external mass bias correction using elements (Eu and Sb) close to cesium masses. The results obtained by the two techniques show good agreement: relative difference on ¹³³Cs/¹³⁷Cs and ¹³⁵Cs/¹³⁷Cs ratios for two nuclear samples, analyzed after chemical separation, ranges from 0.2% to 0.5% depending on the choice of reference value for mass bias correction by MC-ICPMS. Finally the quantification of the ¹³⁵Cs/²³⁸U ratio by the isotope dilution technique is presented in the case of a MOx (mixed oxide) spent fuel sample. Evaluation of the global uncertainties shows that this ratio could be defined at an uncertainty of 0.5% (k = 2). The intercomparison between two independent mass spectrometric techniques is fundamental for the evaluation of uncertainty when no isotopic standard is available.     

Mass selective separation applied to radioisotopes of cesium

A technique that uses the intrinsic mass‐based separation capability of a quadrupole mass spectrometer has been used to resolve spectral radiometric interference of two isotopes of the same element. In this work the starting sample was a mixture of ¹³⁷Cs and ¹³⁴Cs and was (activity) dominated by ¹³⁷Cs. This methodology separated and ‘implanted’ ¹³⁴Cs that was later quantified for spectral features and activity with traditional radiometric techniques. This work demonstrated a ¹³⁴Cs/¹³⁷Cs activity ratio enhancement of >4 orders of magnitude and complete removal of ¹³⁷Cs spectral features from the implanted target mass (i.e. 134). Copyright © 2016 John Wiley & Sons, Ltd.