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.     

Deposition of gamma-emitting nuclides in Japan after the reactor-IV accident at Chernobyl'

The wet and dry deposition of gamma-emitting nuclides are presented for Tsukuba and eleven stations in Japan following the nuclear reactor accident at Chernobyl'. In Japan fallout from the reactor at Chernobyl' was first detected on May 3, 1986, a week after the accident. Abruptly high radioactive deposition, which mainly consists of¹³¹I,¹³²I,¹⁰³Ru,¹³⁷Cs and¹³⁴Cs, was observed in early May. The cumulative amount of¹³¹I,¹⁰³Ru and¹³⁷Cs in May at Tsukuba were 5854±838 Bq·m^–2, 364±54 Bq·m^–2 and 130±26 Bq·m^–2 (decay was corrected to April 26), respectively. The monthly¹³⁷Cs deposition in May corresponds to 2.5% of the cumulative¹³⁷Cs deposition during the period from 1960 through 1982. Most of the Chernobyl' radioactivities, especially¹³¹I, are scavenged from the atmosphere by the wet removal process.     

Thermal neutron cross section and resonance integral of the reaction of135Cs(n,γ)136Cs: Fundamental data for the transmutation of nuclear waste

To determine the cross sections of the¹³⁵Cs(n,γ)¹³⁶Cs reaction, a sample of¹³⁵Cs included in a “standardized solution” of¹³⁷Cs was used as a target and irradiated in a reactor. The ratio of the atom number of¹³⁵Cs to that of¹³⁷Cs was determined to be 0.89±0.03 with a quadrupole mass spectrometer. The thermal cross section and the resonance integral measured in this study were determined to be 8.3±0.3 and 38.1±2.6 b respectively.     

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.     

Radionuclide concentrations in several seaweeds and their annual variations

To examine the radionuclide concentrations in the environment, seaweeds were collected once a year since 1976 at two different places. A marked change was observed in the number of radionuclides in seaweeds. The increase of radionuclides is attributed to contamination by radioactive fallout from Chinese nuclear explosion tests. The radionuclide concentrations were strongly dependent on the species of seaweeds. A gradual decrease of the¹³⁷Cs/⁴⁰K activity ratio was observed in spite of the input of additional¹³⁷Cs fallout from Chinese nuclear tests. This implies that the amounts of¹³⁷Cs introduced into seawater by these detonations were small in comparison with those already contained in seawater. The cesium content in seawater was estimated by using specific activities of¹³⁷Cs in seaweeds and¹³⁷Cs concentration in seawater. The results show good agreement with the reported values by direct analysis of seawater.     

Simultaneous determination of60Co,131I and137Cs in model radioactive waste water by reverse radiometric flow injection analysis with the aid of a multichannel analyzer

Reverse radiometric flow injection analysis was used for the simultaneous determination of⁶⁰Co,¹³¹I and¹³⁷Cs in model radioactive waste water. A NaI (Tl) scintillation detector coupled to a Canberra MCA was used for measuring the activity of¹³⁷Cs at 662 keV,⁶⁰Co at 1173 keV and 1332 keV, and¹³¹I at 364 keV.     

Determination of137Cs,90Sr and fallout Pu in the volcanic soil of Korea

The cumulative depositions of¹³⁷Cs,⁹⁰Sr and fallout Pu in the volcanic ash soil of Korea were determined. The average accumulated depositions of¹³⁷Cs,⁹⁰Sr and fallout Pu in the volcanic soil were much higher than those in other forest sites of Korea. From depth profiles, it was found that¹³⁷Cs,⁹⁰Sr and^239,240Pu in the volcanic soil are more mobile than those in other forest sites of Korea, and that the downward movement of⁹⁰Sr is faster than¹³⁷Cs and^239,240Pu. A significant correlation was found between the concentration of¹³⁷Cs and those of⁹⁰Sr and^239,240Pu. The activity ratios of²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu in soils are close to those observed in the cumulative deposit from the global fallout of nuclear weapon testings.     

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.     

The effect of sorption properties of soil minerals on the vertical migration rate of cesium in soil

The vertical distribution of¹³⁷Cs is shown for two types of soil: silly loamy “supposed” soil and silly lessive one, slightly eroded, occuring in the vicinity of Lublin (Eastern Poland). Based on the distribution data the vertical migration rates of¹³⁷Cs are calculated for both soils. These rates are found to be 0.045 and 0.3 cm/year respectively. The percent contribution of¹³⁷Cs originating from the damaged reactor in Chernobyl is also calculated. The kinetics of cesium adsorption and its adsorption isotherms on minerals separated from the tested soils are also studied. The sorption of Cs on soil minerals markedly affects the migration rate of¹³⁷Cs in soil. The experimental results indicate that, among the extracted mineral fractions, the largest adsorption takes place on marls from the silly loamy soil. This work is supplemented by results of a physicochemical analysis of the studied soils.     

Transfer of137Cs from soil to plants in a wet montane forest in subtropical Taiwan

The distribution of¹³⁷Cs in an undisturbed, multistoried, subtropical wet montane forest ecosystem surrounding Yuanyang Lake (lake surface level ca. 1670m, in northeastern Taiwan), was investigated. The mossy forest here represents a currently-rare perhumid temperate environment in subtropical region. The radioactivity concentration of¹³⁷Cs was determined by γ-spectroscopy with a Ge(Li) detector. Although the soil is extremely acidic (pH 3.3 to 3.6) and the rainfall is high,¹³⁷Cs is evidently retained in the organic layer. The radioactivity concentration of¹³⁷Cs in surface soil ranges from 28 to 71 Bq·kg⁻¹. The concentrations of¹³⁷Cs in the ground moss layer and litter were much lower than that in the soil organic layer, this suggests that¹³⁷Cs detected is not from the newly deposited radioactive fallout. The radioactivity concentration and transfer factor (TF) of¹³⁷Cs varied with plant species. Shrubs and ferns have higher values than a coniferous tree (Taiwan cedar). The TF in this ecosystem is as high as 0.21 to 1.88. The high values of TF is attributed to the abundance of the organic matter in the forest soils. The rapid recycling of¹³⁷Cs through the soil-plant system of this undisturbed multistoried ecosystem suggests the existence of an internal cycling that help the accumulation of¹³⁷Cs in this ecosystem.     

Occurrence of natural radionuclides and fallout cesium-137 in dry-season agricultural land of South Western Nigeria

The radioactivity of the Opa river — irrigated farmlands in the south western Nigeria was determined using an HpGe based, low-level passive gamma-counting system. With the exception of two isotopes, the main radionuclides analysed in the sample were the progenies of²³⁸U and²³²Th. The other two isotopes were the naturally occurring⁴⁰K and the anthropogenic¹³⁷Cs. The result obtained showed elevated levels of radioactivity from all detected radionuclides compared to the published data for this area. Enhanced levels of naturally occurring radionuclides is attributed to the use of phosphatic fertilizers for dry season vegetable cultivation along this river banks. The presence of the fission product¹³⁷Cs could be traced to the fallouts occasioned by the various French nuclear tests in the Sahara desert, and probably, some effect of the more recent nuclear reactor accident at Chernobyl in 1986.     

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.     

Synthesis and characterization of Nb–Ge doped titanosilicate nanoparticles and study of their selectivity for absorption of 137Cs and 90Sr

In this research, for the first time Nb and Ge were doped into titanosilicate nanoparticles up to 25% simultaneously. Crystalline phases and morphology of the synthesized samples were studied by X-ray diffraction (XRD) method and scanning electron microscope (SEM), respectively. Elemental analysis of the samples was performed using X-ray fluorescence (XRF) and Energy dispersive X-ray (EDX) techniques. Surface area of the samples was measured by BET method. Ion exchange potential of the synthesized samples for Sr²⁺ and Cs⁺ and effective parameters such as concentration, temperature, time, and pH were investigated. In addition,¹³⁷Cs and ⁹⁰Sr radio nuclides absorption in the best appropriate sample was examined. The selectivity of the samples for absorption of ¹³⁷Cs and ⁹⁰Sr was studied by gamma spectroscopy, liquid scintillation spectrometry, and atomic absorption spectroscopy methods. The obtained results showed that the prepared samples had good potential for absorption of ¹³⁷Cs and ⁹⁰Sr from the model solution. The sample containing equal amount of niobium and germanium, removed completely the ¹³⁷Cs within the waste water of Tehran nuclear reactor and ⁹⁰Sr in the desired solution.     

Behavior of radiocesium in atmospheric arerosol and fallout in Prague

Radiocesium in ground layer atmospheric aerosol and fallout in Prague has been examined. After a decline in 1986–1988, controlled by a sum of two negative exponentials,¹³⁷Cs aerosol concentration reached a constant level based on an equilibrium between its deposition and resuspension. Deposition velocity was compared to that of⁷Be and²²⁶Ra. It confirmed the supposed source of¹³⁷Cs as resuspension from the ground. Resuspension factor of the order of magnitude of 10^–9 was determined, reminding similar values found earlier in Prague as well as those found in Munich. It also agrees well with the USAEC resuspension model. Solubility of¹³⁷Cs was measured in combined wet and dry fallout. The average undissolved fraction of¹³⁷Cs was found to be about 70% which can be explained by the conditions of the¹³⁷Cs aerosol formation in Chernobyl.     

Natural and artificial radionuclides in soils from Paraná State,Brazil

Soil samples from Paraná State, Brazil, were collected in 1991 and compared with others collected at the same location in March 1977 and at the end of 1983. Pedological analyses were practiced on these samples and¹³⁷Cs and²³²Th,²²⁶Ra and⁴⁰K activities were determined by gammaray spectrometry. A latitude dependence of¹³⁷Cs was found as well. It was impossible to determine the¹³⁷Cs contribution from Chernobyl nuclear accident because of low fallout and intense leaching, erosion and re-suspension in soils of regions with high annual precipitation. Natural radionuclides did not show such effects.     

Determination of90Sr and137Cs in mushrooms following the Chernobyl fallout

After the Chernobyl accident high concentrations of radionuclides were found in Sweden in mushrooms and the contents of⁹⁰Sr and¹³⁷Cs were measured. The level of⁹⁰Sr was generally low and, in proportion to¹³⁷Cs, 2–3 orders of magnitude lower than in the fallut. The contents of¹³⁷Cs varied among species and extreme local variations occurred. The ratio¹³⁴Cs/¹³⁷Cs diverged from other biological samples leading to the conclusion that old fallout was involved in the uptake.     

Removal of226Ra(II) from uranium mining and processing effluents

The activity of¹³⁷Cs was determined in mosses and their surrounding soils in three Venezuelan cloud forests. The concentration of¹³⁷Cs in both the mosses and their respective soils were correlated with elevation (m.a.s.l.). This relationship was the result of the cloud forest effect, no direct deposition by condensation below the base of the clouds and increasing deposition of¹³⁷Cs with the density of the clouds. The ratio of the activity of¹³⁷Cs in the mosses to their surrounding soils was in general the same for sites near the top of the mountains, but the ratio at the Altos de pipe location was 3.5 times higher than that of the La Sierra mountain. This was explained by the difference in the water content of the surface and the top soil layer. It was concluded that the¹³⁷Cs measured in the mosses was from the soil effect rather than new deposition of¹³⁷Cs in the last three years.     

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.     

Temporal variations of137Cs concentrations in the surface seawater and marine organisms collected from the Japanese coast during the 1980's

The surface seawater and marine organisms were collected on the Japanese coast and analyzed for their¹³⁷Cs concentrations during the 1980's. The¹³⁷Cs concentrations in surface seawater decreased almost exponentially with time and the¹³⁷Cs removal rate constant was estimated to be 0.0445 y⁻¹. The¹³⁷Cs concentrations in marine organisms also decreased almost exponentially with time. The environmental half-lives of¹³⁷Cs in muscle and viscera of fish, crustacea, and seaweed were estimated from the measured decreases of¹³⁷Cs concentrations.     

Leaching behavior of137Cs in cement

To assess the safety of disposal of a radioactive waste-cement composite, the leaching of¹³⁷Cs from a waste composite into a surrounding fluid has been studied. Leaching tests were carried out in accordance with a method recommended by IAEA.¹ The leachability was measured as a function of bentonite clay to cement ratio. The fraction of¹³⁷-Cs leached from a specimen of Portland cement is 0.03–0.13 at a leaching time of 400 d. Results presented in this paper are examples of data obtained in a 10 y mortar and concrete testing project, which will influence the design of the engineered trench system for a future Yugoslav radioactive waste storage center.^2,3