Cesium isotope ratios as indicators of nuclear power plant operations

There are multiple paths by which radioactive cesium can reach the effluent from reactor operations. The radioactive ¹³⁵Cs/¹³⁷Cs ratios are controlled by these paths. In an effort to better understand the origin of this radiation, these ¹³⁵Cs/¹³⁷Cs ratios in effluents from three power reactor sites have been measured in offsite samples. These ratios are different from global fallout by up to six fold and as such cannot have a significant component from this source. A cesium ratio for a sample collected outside of the plant boundary provides integration over the operating life of the reactor. A sample collected inside the plant at any given time can be much different from this lifetime ratio. The measured cesium ratios vary significantly for the three reactors and indicate that the multiple paths have widely varying levels of contributions. There are too many ways these isotopes can fractionate to be useful for quantitative evaluations of operating parameters in an offsite sample, although it may be possible to obtain limited qualitative information for an onsite sample.     

Fixation of Cs to marine sediments estimated by a stochastic modelling approach

Dumping of nuclear waste in the Kara Sea represents a potential source of radioactive contamination to the Arctic Seas in the future. The mobility of 137Cs ions leached from the waste will depend on the interactions with sediment particles. Whether sediments will act as a continuous permanent sink for released 137Cs, or contaminated sediments will serve as a diffuse source of 137Cs in the future, depends on the interaction kinetics and binding mechanisms involved. The main purpose of this paper is to study the performance of different stochastic models using kinetic information to estimate the time needed for Cs ions to become irreversibly fixed within the sediments. The kinetic information was obtained from 134Cs tracer sorption and desorption (sequential extractions) experiments, conducted over time, using sediments from the Stepovogo Fjord waste dumping site, on the east coast of Novaya Zemlya. Results show that 134Cs ions interact rapidly with the surfaces of the Stepovogo sediment, with an estimated distribution coefficient Kd(eq) of 300 ml/g (or 13m2/g), and the 134Cs ions are increasingly irreversibly fixed to the sediment over time. For the first time, stochastic theory has been utilised for sediment-seawater systems to estimate the mean residence times (MRTs) of Cs ions in operationally defined sediment phases described by compartment models. In the present work, two different stochastic models (i) a Markov process model (MP) being analogous to deterministic compartment models, and (ii) a semi-Markov process model (SMP) which should be physically more relevant for inhomogeneous systems, have been compared. As similar results were obtained using the two models, the less complicated MP model was utilised to predict the time needed for an average Cs ion to become irreversibly fixed in the Stepovogo sediments. According the model, approximately 1100 days of contact time between Cs ions and sediments is needed before 50% of the 134Cs ion becomes fixed in the irreversible sediment phase. while about 12.5 years are needed before 99.7% of the Cs ions are fixed. Thus, according to the model estimates the contact time between 137Cs ions leached from dumped waste and the Stepovogo Fjord sediment should be about 3 years before the sediment will act as an efficient permanent sink. Until then a significant fraction of 137Cs should be considered mobile. The stochastic modelling approach provides useful tools when assessing sediment-seawater interactions over time, and should be easily applicable to all sediment-seawater systems including a sink term.     

Depositional records of plutonium and (137)Cs released from Nagasaki atomic bomb in sediment of Nishiyama reservoir at Nagasaki

In a sediment core of Nishiyama reservoir at Nagasaki city, depth profiles of (240)Pu/(239)Pu isotopic ratio, (239+240)Pu and (137)Cs activities were determined. Sediments containing plutonium and (137)Cs, which were deposited immediately after a detonation of Nagasaki atomic bomb, were identified in the core. Observed below the sediments were macroscopic charcoals, providing evidence for initial deposit of the fallout of the Nagasaki atomic bomb. This is the first entire depositional records of plutonium and (137)Cs released from the Nagasaki atomic bomb together with those from atmospheric nuclear tests.     

Radioactivity concentrations of 40K, 134Cs, 137Cs, 90Sr, 241Am, 238Pu and 239+240Pu radionuclides in Jordanian soil samples

In November 2000, surface and core soil samples were collected from different regions of Jordan. The samples were analyzed by direct gamma spectrometry and combined radiochemical separation procedure to quantify (40)K, (134)Cs, (137)Cs, (90)Sr, (241)Am, (238)Pu and (239+240)Pu radioactivity. Concentrations (Bq.kg(-1) dry weight) have been observed to vary in the range 1.5-2.6 for (134)Cs, 2.8-11.4 for (90)Sr, and 0.13-0.48 for (241)Am, 0.016-0.062 for (238)Pu, 0.28-1.01 for (239+240)Pu and 155-543 for (40)K. The typical concentration of (137)Cs found in topsoils (0-2 cm) ranged in 7.5-576 Bq.kg(-1), dry weight. These values were greater than those observed in samples taken at greater depths (up to 32 cm). Activity ratios of (134)Cs/(137)Cs, (90)Sr/(137)Cs, (239+240)Pu/(137)Cs, (238)Pu/(137)Cs, (241)Am/(137)Cs, (239+240)Pu/(238)Pu and (241)Am /(238)Pu have mean values of 0.0049 (R=1), 0.29 (R=0.76), 0.41 (R=0.90), 0.39 (R=0.85), 0.41 (R=0.88), 7.72 (R=0.97) and 16.66 (R=0.98), respectively. The underlying concentrations were correlated and relatively higher than those reported in neighboring countries. One moss sample, as a biomonitor indicator, was measured and evaluated along with the soil samples. Its data showed higher concentrations of all measured radionuclides due to accumulations over years. The depth distribution of the fission product (137)Cs and the total deposition (Bq.m(-2)) were also studied in selected samples. Estimations of the annual effective dose equivalent due to (137)Cs-soil contamination showed values up to more than 200 microSv.     

Distribution of 137Cs in soil along Ta-han River Valley in Tau-Yuan County in Taiwan

Environmental 137Cs contamination was suspected from accidents at spent fuel storage pits of a research reactor site in the Ta-han River valley in Taiwan. In order to further characterize this contamination, soil samples were collected and measured by a gamma-spectroscopy system in 1999. It was found that 137Cs contamination is distributed up to 4 km from the reactor in an area covered mostly by rice and plant fields. 137Cs concentration in the topsoil ranged up to about 1000 Bq kg-1, as compared with soil beyond the contaminated area, which does not exceed 15 Bq kg-1. Spatial distribution of 137Cs was characterized by strong non-uniformity, which complicated our understanding of the distribution pathway of the radionuclides. The highest concentrations of 137Cs, up to more than 1000 Bq kg-1, were found within a few rice fields. The relative location of these rice fields and the water supplies from local streams suggested that the 137Cs was distributed along water pathways in the valley.     

Comparison of Pu and (137)Cs as tracers of soil and sediment transport in a terrestrial environment

Following atmospheric nuclear weapons testing in the 1950s and 1960s significant quantities of (137)Cs and (239+240)Pu were deposited worldwide. In recent decades, (137)Cs has been commonly used as a tracer of soil erosion and sedimentation, particularly in the Northern Hemisphere where atomic deposition was three times as great as in the Southern Hemisphere. The relatively short 30-year half-life of this isotope means that its sensitivity as a tracer is rapidly decreasing. In contrast, with half-lives of 24,110 and 6561 years, the sensitivity of the two plutonium isotopes remains essentially the same as when it was deposited. Here we use the technique of Accelerator Mass Spectrometry to demonstrate the potential of anthropogenic Pu as an alternative to (137)Cs as a tracer of soil transport in Australia. We measure an average (137)Cs/(239+240)Pu activity ratio of 27.3+/-1.5 and an average (240)Pu/(239)Pu atom ratio of 0.149+/-0.003, both slightly lower than the global average.     

Radionuclide tracing of water masses and processes in the water column and sediment in the Algerian Basin

Caesium-137 and (239,240)PU were analysed in the water column along the Algerian coast. The (137)Cs activity concentration in surface water increased from the west to the east from 1.6 to 3.3 mBq L(-1), documenting a presence of Modified Atlantic Water (MAW) in the region. Higher concentrations observed in deep waters may be due to an intrusion of Levantine Intermediate Water (LIW), which has been carrying higher levels of (137)Cs from Chernobyl accident. The (239,240)Pu sub-surface concentration peaked at about 250 m water depth as a result of biogeochemical processes in the water column. The observed (239,240)Pu/(137)Cs activity ratio at the surface (0.003) was significantly lower than that in global fallout (0.04). This decrease exceeds that expected from radioactive decay of (137)Cs, and confirms that Pu due to its adsorption on sinking particles is more effectively removed from surface layers than is (137)Cs. An increase of the (239,240)Pu/(137)Cs activity ratio with depth suggests that (239,240)Pu, similarly as (137)Cs, should be also transported by advection to maintain the observed ratios in deep waters. An intrusion of LIW may enhance therefore both the (137)Cs and (239,240)Pu concentrations in deep waters. The average (238)Pu/(239+240)Pu activity ratio in seawater was 0.03+/-0.02, confirming a global fallout origin of Pu in the Algerian Basin. Caesium-137 and (239,240)Pu inventories in the water column were estimated to be from 2.7+/-0.5 kBq m(-2) to 3.8+/-0.7 kBq m(-2), and from 13.8+/-2.6 Bq m(-2) to 41+/-7B qm(-2), respectively. The (137)Cs massic activities in surface sediment were almost constant, the average activity was 9.0+/-0.8 Bq kg(-1). Sedimentation rates obtained using the (210)Pb method were from 0.1 to 0.7 cm y(-1), and resulting penetration depths of (137)Cs in the sediment cores were from 15 to over 40 cm. The (137)Cs peaks found in the sediment cores were associated with the Chernobyl accident (1986) and global fallout (1964). The (137)Cs inventories in the sediment were increasing from the west (180 Bq m(-2)) to the east (350 Bq m(-2)).     

Activity ratios of 137Cs, 90Sr and 239+240Pu in environmental samples

Both global and Chernobyl fallout have resulted in environmental contamination with radionuclides such as 137Cs, 90Sr and 239+240Pu. In environmental samples, 137Cs and 239+240Pu can be divided into the contributions of either source, if also the isotopes 134Cs and 238Pu are measurable, based on the known isotopic ratios in global and Chernobyl fallout. No analogous method is available for 90Sr. The activity ratios of Sr to Cs and Pu, respectively, are known for the actual fallout mainly from air filter measurements; but due to the high mobility of Sr in the environment, compared to Cs and Pu, these ratios generally do not hold for the inventory many years after deposition. In this paper we suggest a method to identify the mean contributions of global and Chernobyl fallout to total Sr in soil, sediment and cryoconite samples from Alpine and pre-Alpine regions of Austria, based on a statistical evaluation of Sr/Cs/Pu radionuclide activity ratios. Results are given for Sr:Cs, Sr:Pu and Cs:Pu ratios. Comparison with fallout data shows a strong depletion of Sr against Cs and Pu.     

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland)

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.     

Use of 129I and 137Cs in soils for the estimation of 131I deposition in Belarus as a result of the Chernobyl accident

Using radioactivity measurements for 131I and 137Cs and nuclear activation analysis (NAA) or accelerator mass spectrometry (AMS) for 129I, ratios of 131I/137Cs and 129I/137Cs have been determined in soils from Belarus. We find that the pre-Chernobyl ratio of 129I/137Cs in Belarus is significantly larger than expected from nuclear weapons fallout. For the Chernobyl accident, our results support the hypothesis that there was relatively little fractionation of iodine and caesium during migration and deposition of the radioactive cloud. For sites having 137Cs > 300 Bq/kg, 129I can potentially give more reliable retroactive estimates of Chernobyl 131I deposition. However, our results suggest that 137Cs can also give reasonably good (+/-50%) estimates for 131I in Belarus.     

Long-term flux of Chernobyl-derived 137Cs from soil to French rivers: a study on sediment and biological indicators

Sediment and aquatic plants were collected annually since the early 1990s in the main French rivers, upstream of nuclear power plants. These time series were used in order to assess the parameters of a compartmental model describing the Chernobyl-derived (137)Cs flux from soil to rivers. In order to reduce the dispersal of (137)Cs measured activities in sediment samples due to the granulometric heterogeneity, a correction method was set up using sediment test-fractions artificially enriched with specific diameter particles. The method was based on (137)Cs affinity for fine particles, especially clays, and thus clay and fine silt contents of each sample was analysed. Corrected sediment data showed (1) that the method efficiently reduced the variability; and (2) that (137)Cs activities in French rivers decreased with a half-life of 4 to 6 years since 1987 (after correction by radioactive decay). A similar half-life value was obtained for aquatic plants pointing out that this half-life is related to the gradual decay of the flux from soil to rivers, not to the indicator itself. Comparing our results with similar ones published by other authors, it appeared possible that this kinetic varies with the time period over which the study is conducted, the longer the period the lower is the kinetic.     

238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in soils around nuclear research centre Rez, near Prague

Forty-four soil samples were taken around the nuclear research centre Rez, near Prague. The mean activity concentrations of 238Pu, 239,240Pu, 241Am, 90Sr and 137Cs in uncultivated soil were 0.010, 0.26, 0.12, 2.7 and 23 Bq.kg(-1), respectively. Contents of radionuclides in cultivated soil were lower and in forest soil higher than in uncultivated soil. The mean activity ratios of 238Pu/239,240Pu, 241Am/239,240Pu, 90Sr/239,240Pu and 239,240Pu/137Cs in uncultivated soil were 0.041, 0.47, 10.9 and 0.013, respectively. The mean activity ratios in cultivated and forest soils were close to the values given above. It follows from the results that the source of 239,240Pu, 90Sr and 137Cs in the studied area is deposition from atmospheric nuclear tests, in the case of 137Cs also deposition from Chernobyl accident. The contribution of the research centre effluents was not proved for these radionuclides. Increased activity ratio of 241Am/239,240Pu indicates the presence of 241Am in the soils studied emanating from sources other than nuclear tests. Uniform distribution of the 241Am/239,240Pu activity ratio around the nuclear research centre and the absence of an area with evidently higher activity ratio, including at sites lying in the main wind direction, suggest that the additional activity of 241Am does not originate from the nuclear research centre. The additional source might be the deposition following the Chernobyl accident.     

Residual radioactive contamination at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" in the Republic of Sakha (Yakutia)

In this paper, results are reported on the concentrations and activity ratios of 137Cs, 239+240Pu and 238Pu in soils, lichen and bottom sediments collected at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" (Republic of Sakha (Yakutia), North-East Siberia). At the "Craton-3" site, 239- 240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g in surface soils (0-5 cm) and 239+240Pu concentrations up to 7.4 Bq/g in lichen were observed. The 137Cs concentration in measured soils range from 0.52 to 216 Bq/g for the near-plume and from 1.65 to 21.5 Bq/g for the far-plume. In lichen, 137Cs concentration varied from a global background level up to 251 Bq/g. Radioactive contamination at "Crystal" demonstrates an extremely irregular distribution of 239,240Pu and 137Cs in environmental samples taken at locations within 150 m radius of the site. Further work on compiling detailed maps of radioactive contamination of the territory around "Craton-3" and "Crystal" is discussed.     

Assessment of the genotoxicity of 137Cs radiation using Vicia-micronucleus, Tradescantia-micronucleus and Tradescantia-stamen-hair mutation bioassays

Since the middle of the 20th century, ionizing radiations from radioactive isotopes including 137Cs have been investigated to determine their genotoxic impact on living organisms. The present study was designed to compare the effectiveness of three plant bioassays to assess DNA damage induced by low doses of 137Cs: Vicia-micronucleus test (Vicia-MCN), Tradescantia-micronucleus test (Trad-MCN) and Tradescantia-stamen-hair mutation test (Trad-SH) were used. Vicia faba (broad bean) and Tradescantia clone 4430 (spiderwort) were exposed to 137Cs according to different scenarios: external and internal (contamination) irradiations. Experiments were conducted with various levels of radioactivity in solution or in soil, using solid or liquid 137Cs sources. The three bioassays showed different sensitivities to the treatments. Trad-MCN appeared to be the most sensitive test (significative response from 1.5 kBq/200 ml after 30 h of contamination). Moreover, at comparable doses, internal irradiations led to larger effects for the three bioassays. These bioassays are effective tests for assessing the genotoxic effects of radioactive 137Cs pollution.     

Evidence of the radioactive fallout in the center of Asia (Russia) following the Fukushima Nuclear Accident

It was recently reported that radioactive fallout due to the Fukushima Nuclear Accident was detected in environmental samples collected in the USA and Greece, which are very far away from Japan. In April-May 2011, fallout radionuclides (¹³⁴Cs, ¹³⁷Cs, ¹³¹I) released in the Fukushima Nuclear Accident were detected in environmental samples at the city of Krasnoyarsk (Russia), situated in the center of Asia. Similar maximum levels of ¹³¹I and ¹³⁷Cs/¹³⁴Cs and ¹³¹I/¹³⁷Cs ratios in water samples collected in Russia and Greece suggest the high-velocity movement of the radioactive contamination from the Fukushima Nuclear Accident and the global effects of this accident, similar to those caused by the Chernobyl accident.     

Deposition of 137Cs in Rokkasho, Japan and its relation to Asian dust

Biweekly atmospheric depositions of (137)Cs were measured in Rokkasho, Aomori, Japan from March 2000 to March 2006 to study recent (137)Cs deposition. Although the deposition level was generally lower than the detectable limit, deposition samples collected in spring occasionally had measurable levels of (137)Cs. The annual (137)Cs deposition from 2001 to 2005 was 0.04-0.69 Bq m(-2) with a mean value of 0.27 Bq m(-2). Depositions of insoluble Al, Fe and Ti were strongly correlated with the (137)Cs deposition, suggesting that suspension of soil particles was the main source of the recent (137)Cs deposition. Asian dust events were coincident with some of the significant (137)Cs depositions in spring. It was found that the ratios of (137)Cs/Al and Fe/Al could be used as indices for discriminating Asian dust from suspension of the local surface soil. Backward trajectory analysis suggested southern Mongolian and northeastern China regions as sources of the significant (137)Cs depositions.     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides ((90)Sr, (137)Cs and (239+240)Pu) in seabed sediment in the Japan Sea were collected during the period 1998-2002. Concentration of (90)Sr, (137)Cs and (239+240)Pu in seabed sediment was 0.07-1.6 Bq kg(-1), 0.4-9.1 Bq kg(-1) and 0.002-1.9 Bq kg(-1), respectively. In the northern basin of the sea (Japan Basin), (239+240)Pu/(137)Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher (239+240)Pu/(137)Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38 degrees N), both inventories and (239+240)Pu/(137)Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

Determination of extremely low (236)U/(238)U isotope ratios in environmental samples by sector-field inductively coupled plasma mass spectrometry using high-efficiency sample introduction

A method by inductively coupled plasma mass spectrometry (ICP-MS) was developed which allows the measurement of (236)U at concentration ranges down to 3 x 10(-14)g g(-1) and extremely low (236)U/(238)U isotope ratios in soil samples of 10(-7). By using the high-efficiency solution introduction system APEX in connection with a sector-field ICP-MS a sensitivity of more than 5,000 counts fg(-1) uranium was achieved. The use of an aerosol desolvating unit reduced the formation rate of uranium hydride ions UH(+)/U(+) down to a level of 10(-6). An abundance sensitivity of 3 x 10(-7) was observed for (236)U/(238)U isotope ratio measurements at mass resolution 4000. The detection limit for (236)U and the lowest detectable (236)U/(238)U isotope ratio were improved by more than two orders of magnitude compared with corresponding values by alpha spectrometry. Determination of uranium in soil samples collected in the vicinity of Chernobyl nuclear power plant (NPP) resulted in that the (236)U/(238)U isotope ratio is a much more sensitive and accurate marker for environmental contamination by spent uranium in comparison to the (235)U/(238)U isotope ratio. The ICP-MS technique allowed for the first time detection of irradiated uranium in soil samples even at distances more than 200 km to the north of Chernobyl NPP (Mogilev region). The concentration of (236)U in the upper 0-10 cm soil layers varied from 2 x 10(-9)g g(-1) within radioactive spots close to the Chernobyl NPP to 3 x 10(-13)g g(-1) on a sampling site located by >200 km from Chernobyl.     

Estimating the date corresponding to the horizon of the first detection of 137Cs and 239+240Pu in sediment cores

The anthropogenic bomb fallout nuclides 137Cs and plutonium isotopes (240Pu, 239Pu) are important chronometers for the determination of recent sediment accumulation rates using sediment cores collected from various water bodies. One of the crucial time horizons used to date sediment core profiles corresponds to the date of first detection of these nuclides. Although atmospheric nuclear testing began during the mid-1940s, the year corresponding to a nuclide's first detection when measured in 2006 depends on a number of factors including fallout history, radioactive half-life, gamma/alpha detection limits, geographic latitude and the accumulated thickness of the sediment section. This paper reports estimations of the year of first detection in sediment profiles of fallout 137Cs and Pu measured by gamma and alpha spectrometry, respectively. We find that for the latitude 30-40 degrees south of the equator the year of first detection for 137Cs is 1955. The date is earlier in the northern hemisphere due to higher fallout rates. Due to better measurement sensitivity first detection of Pu is generally earlier than 137Cs by 1-2 years.     

137Cs contamination in tea and yerba mate in South America

Gamma-ray spectra from more than 50 samples of food products available in stores of Buenos Aires city were measured using a germanium detector. Activity concentrations of 137Cs up to 10 Bq/kg were found in tea and yerba mate manufactured in Apóstoles, Argentina. Further measurements of tea leaves, yerba mate leaves and soils, all coming from a cultivated area in that region, also show the presence of 137Cs contamination. The results suggest that the area was fertilized with a product that originated in a region affected by the fallout from the Chernobyl nuclear plant accident.