Monitoring the environmental contamination of Kara Sea and shallow bays of Novaya Zemlya

The distribution of ¹³⁷Cs and ^239,240Pu in various ecosystems of the Kara Sea as well as speciation of these radionuclides has been studied to assess their potential mobility. In bottom sediment and seawater samples collected in Abrosimov, Tsivolky, Stepovoy, and Sedov Bays and on the coast of Novaya Zemlya, the content of anthropogenic radionuclides ¹³⁷Cs and ^239,240Pu does not exceed the values typical of the offshore zone in the Kara Sea (in sea water: 1.0–3.7 Bq/m³ for ¹³⁷Cs and 50–90 mBq/m³ for ^239,240Pu; in bottom sediments: 0.5–18.3 Bq/kg for ¹³⁷Cs and 4.3–7.3 Bq/kg for ^239,240Pu). The present monitoring study is important for the development of a long-term forecast for the dynamics of environmental contamination in the shallow bays of Novaya Zemlya.     

Current levels and distribution of 137Cs and Pu isotopes in soil on the Kazakhstan territory of the Kazakhstan-Chinese border: Semipalatinsk and Lob Nor nuclear test sites detonation

More than 100 soil samples were collected from 46 sites along roads and some settlements connecting Alma-Ata to Semipalatinsk City of the Kazakhstan-Chinese border and analyzed for ¹³⁷Cs and Pu isotopes (²³⁸Pu, ²³⁹Pu and ²⁴⁰Pu). The mean ¹³⁷Cs inventory at each site was within the range of 1,000-3,000 Bq/m² for most of the sites. The ^239,240Pu concentration and its inventories were observed in the wide range of 0.18-2.6 Bq/kg and 28-677 Bq/m², respectively. At the most northern sites in the areas studied, higher^239,240Pu inventories were found corresponding to the increase of ^239,240Pu fraction which was not leached by hot digestion with conc. HNO₃+H₂O₂. The ^239,240Pu/¹³⁷Cs activity ratios for the soil samples from the southern areas lie in the narrow range of 0.016–0.039 (most of data being 0.02–0.03), probably indicative of global fallout origin. On the other hand, a little or several higher ratios (0.05 to 0.22) were found for soil samples from the northern areas. These higher ratios demonstrate strongly that there was additional Pu input of local fallout due to the atomic explosions. From ²⁴⁰Pu/²³⁹Pu atomic ratios measured, contribution of local fallout ^239,240Pu, probably from the SNTS, was found to be higher (60–86%) in the sites around the northern areas than the southern ones. The present data might serve not only as a current baseline information on distribution and contamination levels of the long-lived fallout radionuclides in the Kazakhstan areas of the Kazakhstan-Chinese border, but also as a aid of selection of control area for epidemiological projects.     

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.     

Some aspects of environmental radioactivity around the former Soviet Union"""s Semipalatinsk nuclear test site: Local fallout Pu in Ust"""-Kamenogorsk district

The ¹³⁷Cs, ²³⁸Pu and ^239,240Pu activity concentrations were determined together with the atomic ratios of ²⁴⁰Pu/²³⁹Pu for the soil samples at 19 sites from the Ust"-Kamenogorsk district, located more than 300 km east of the Semipalatinsk nuclear test site (SNTS). The mean areal deposition of ¹³⁷Cs ranged from 1,500 to 4,100 Bq/m². However, some hot spot-like areas showing high concentrations of 5,500–7,700 Bq/m² were foundat some sites within the city. The ^239,240Pu levels ranged from <50 to 510 Bq/m², however most of them ranged between 120–200 Bq/m². These levels are nearly the same as those around the Semipalatinsk City. At most of the sites within the city and its adjacent areas, both nuclides were found in the soil layers up to a depth of 30 cm. A fraction of 20–50% of ^239,240Pu was not leached by hot digestion with concentrated HNO₃ containing a small amount of H₂O₂. Generally, such tightly bound fraction showed a trend to decrease with increasing distance from the SNTS. The fraction of these radionuclides that were deposited in Ust"-Kamenogorsk district from global and from SNTS fallouts have been determined using the ²⁴⁰Pu/²³⁹Pu atomic ratios in both Pu fractions: one which can be leached with hot HNO₃ + H₂O₂ and another that is a non-leacheable for each soil layer of core samples. As a result a fraction of 21–80% (mostly 30–60%) of total ^239,240Pu were found to be due to the local fallout of Pu from the SNTS debris. For ¹³⁷Cs, the contribution (mostly 10–20%) of local fallout from the SNTS were estimated to be far lower as compared to ^239,240Pu.     

Distributions of Pu isotopes and 137Cs in soil from Semipalatinsk Nuclear Test Site detonations throughout southern districts

Soil samples collected mainly from the southern areas, including Kainar and Karaul settlements, around the Semipalatinsk Nuclear Test Site of the former USSR were analyzed for ¹³⁷Cs and Pu isotopes (²³⁸Pu,²³⁹Pu and ²⁴⁰Pu) by γ-ray and α-ray spectrometry and ICP-MS. The ¹³⁷Cs inventories varied widely from 170 to 13,600 Bq/m². The ^239,240Pu inventories, values of which are scare in the literature, also varied in the range of 34-2,050 Bq/m² (most of date being 100-300 Bq/m²). In the areas around Tailan, Sarzal and Karaul settlements where the radioactive cloud related to the first thermonuclear explosion passed through, higher inventories of these nuclides were observed and especially their ²³⁸Pu/^239,240Pu activity ratios (0.0064-0.0076) were markedly lower than those attributed to global fallout (0.03-0.04). The observed ratios might be used as a fingerprint to identify the Pu source of the first thermonuclear event. Most of the ²⁴⁰Pu/²³⁹Pu atomic ratios were lower than those of global fallout (0.18) commonly accepted. The contribution of local fallout ^239,240Pu was higher (more than 80-90%) in the areas around the Tailan, Sarzal and Karaul settlements than that (30-ca. 60%) in the other areas. This high Pu contribution was related to the Pu source from the first thermonuclear event. This revised version was published online in July 2006 with corrections to the Cover Date.     

Plutonium isotopes and 137Cs in Dolon settlement near the Semipalatinsk Nuclear Test Site: About 50 years after the first nuclear weapon testing

Recent controversies concerning the radiation doses for populations living in the village of Dolon due to the nuclear explosions carried out at the Semipalatinsk Nuclear Test Site (SNTS) have encouraged us to evaluate in more detail the levels and distributions of residual long-lived radionuclides¹³⁷Cs and Pu isotopes (²³⁸Pu,^239,240Pu) in soils within the village. Soil core samples up to a depth of about 30 cm and/or 100 cm were collected at 25 sites and subjected to analysis of ¹³⁷Cs and Pu isotopes. The inventories of ¹³⁷Cs and ^239,240Pu were found to be in the wide range of 790-10,310 and 530-14,320 Bq/m², respectively. Sequential leaching of Pu from the soil showed that more than ca. 80% of the ^239,240Pu was not leached by hot digestion with conc. HNO³ + H₂O₂, indicating the presence of Pu associated with fused silicates. Further, the presence of hot-particles from the Pu contaminants by a-track radiography technique using CR-39 polycarbonate was confirmed in the soil, even at present, after about 50 years from the first nuclear weapon testing. This revised version was published online in July 2006 with corrections to the Cover Date.     

Pu isotopes and137Cs in the surrounding areas of the former Soviet Union's Semipalatinsk nuclear test site

Field missions were sent to Semipalatinsk City and several settlements near the former Semipalatinsk nuclear test site to investigate the current radioactive contamination levels of the land coming from long-lived radionuclides. The soil was sampled at about 20 sites, including some settlements such as Mostik, Dolon and Chagan, forest and pasture areas, along the roads from Semipalatinsk City to Kurchatov City and to Korosteli settlement in the direction of the Altai District. The radioactivities of¹³⁷Cs,²³⁸Pu and^239,240Pu as well as²⁴⁰Pu/²³⁹Pu atomic ratios in the soil were determined by non-destructive γ-ray spectrometry and radiochemical separation followed by α-ray spectrometry and/or ICP-MS, respectively. The results showed a distinction of¹³⁷Cs and^239,240Pu inventories in soil depending on the site where we visited. While the overall¹³⁷Cs levels were as same as or slightly lower than the domestic global fallout level (3·10³–7·10³ Bq/m²),^239,240Pu levels at some sites were several to a few ten times higher than the domestic level (40–120 Bq/m²). The atomic ratios of²⁴⁰Pu/²³⁹Pu in the soil were in the range of 0.024–0.125, which were significantly lower than the value of 0.18 commonly accepted for global fallout Pu.     

Results of three years of monitoring239,240Pu and238Pu concentrations in airborne effluents from the V-1 nuclear power plant with VVER 440 reactors in Jaslovské Bohunice in Czechoslovakia

The concentration of^239,240Pu and²³⁸Pu in airborne effluents in the years 1985–1987 from two reactors VVER 440/total power of 880 MW/ of a nuclear power plant V-1 in Jaslovské Bohunice in Czechoslovakia, was determined. The concentration of^239,240Pu in effluents ranged from 1.0 to 30.8 Bq.m^–3 and of²³⁸Pu from 1.6 to 41.1 Bq.m^–3. The activity ratio²³⁸Pu/^239,240Pu in airborne effluents kept within the range of 1.0–2.4. Total annual discharged activities of^239,240Pu in 1985, 1986 and 1987 were 28.5, 12.7 and 12.2 kBq, respectively. Total annual discharged activities of²³⁸Pu in 1986 and 1987 were 16.6 and 15.1 kBq, respectively.     

Anomalously high237Np in intertidal sediments from the Ribble Estuary in the Irish Sea

Depth profiles and inventories of²³⁷Np in sediment cores from the Ribble Estuary in the Irish Sea have been studied along with those of Pu isotopes,²⁴¹Am and¹³⁷Cs, to allow a more detailed look of anomalously high²³⁷Np content observed in this estuary previously. The comprehensive data obtained showed that the depth profiles of both²³⁷Np contents and²³⁷Np/^239,240Pu activity ratios were clearly different from those of^239,240Pu,²⁴¹Am, and¹³⁷Cs and their activity ratios. As much as 80–90% of²³⁷Np inventories (0.32–1.06 kBq/m²), found in three cores, were estimated to be derived from a source other than Sellafield, on the basis of comparison of the²³⁷Np/^239,240Pu inventory ratio (0.65–1.74%) found in the Ribble Estuary cores with those (0.10–0.16%) in the Ravenglass Estuary cores.     

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.     

Cs, Am and Pu isotopes as tracers of sedimentation processes in the Curonian Lagoon–Baltic Sea system

¹³⁷Cs, ²⁴¹Am and Pu isotopes were analyzed in seawater, bottom sediments (BS) and suspended particulate matter samples collected in the Baltic Sea during 1997–2011. The particle size distribution and sequential extraction studies were carried out with the aim to better understand the association of radionuclides with particles and their bonding patterns in the BS. δ¹³C_org was applied for identification of sources of organic matter in the studied area. It has been found that massic activities of ¹³⁷Cs in BS varied from 2.1 to 588 Bq/kg. High correlation of ¹³⁷Cs massic activities with total organic carbon (TOC) in BS (r = 0.75) and with clay minerals (r = 0.95) was found. ^239,240Pu massic activities in BS varied from 0.03 to 7.5 Bq/kg. High correlation with TOC was found for ^239,240Pu (R = 0.98) as well as for ²⁴¹Am (r = 0.96). δ¹³C_org in the studied samples ranged from ?22.3 to ?31.8 ‰.     

239,240Pu,241Am and137Cs in soils from several areas in China

This paper gives the first data on^239,240Pu and²⁴¹Am in Chinese soils. Surface soil samples with a set of 0–5 cm and 5–20 cm depth were collected from Beijing, Taiyuan, Shijiazhuang and Jinang of China in 1990, and^239,240Pu,²⁴¹Am and¹³⁷Cs, including naturally occurring radionuclides, in these samples were measured to evaluate their present levels and distributions. From these results, the average accumulated depositions were estimated roughly to be 24±13 MBq/km² for^239,240Pu, 10±5 MBq/km² for²⁴¹Am and 1.2±0.7 GBq/km² for¹³⁷Cs. The activity ratios of^239,240Pu/¹³⁷Cs and²⁴¹Am/^239,240Pu ranged from 0.016 to 0.026 with a mean value of 0.020±0.004 and 0.35 to 0.49 with a mean value of 0.43±0.05, respectively.     

Plutonium isotopes in the Sea of Japan

Plutonium isotopes in the Sea of Japan were determined to assess radioactive contamination. Concentrations of ^239,240Pu in surface water of the Sea of Japan were maintained at a constant level over the past two decades in contrast to ¹³⁷Cs. A median value of surface ^239,240Pu in the Sea of Japan in this period was 5.6 mBq/m³ with the range between 2.1 and 14.0 mBq/m³, which is slightly higher than that in the western North Pacific. The vertical distribution of ^239,240Pu showed a surface minimum, a subsurface maximum and gradual decrease with increasing depth. The ²⁴¹Pu/^239,240Pu activity ratios in water columns were almost constant except for surface water. In regard to ^239,240Pu in surface water of the Sea of Japan, these findings suggest that rapid recycling of deeper plutonium occurs in the Sea of Japan due to deep convection in winter and biogeochemical processes such as particle scavenging and remineralization.     

238Pu, 239+240Pu, 241Am, 90Sr and 137Cs in mountain soil samples from the Tatra National Park (Poland)

Activity concentrations and inventory for ²³⁸Pu, ^239+240Pu, ²⁴¹Am, ⁹⁰Sr, and ¹³⁷Cs in soil from Tatra Mountains of Poland are presented. Soil samples were collected using 10 cm diameter cores down to 10 cm and sliced into 3 slices. Details of the applied procedure are described with the quality assurance program. The maximum activity concentrations found for various samples were: 1782±13 Bq/kg, 17.4±0.9 Bq/kg, 3.4±0.3 Bq/kg and 84±7 Bq/kg for ¹³⁷Cs, ^239+240Pu, ²⁴¹Am and ⁹⁰Sr, respectively. The maximum cumulated deposition of ^239+240Pu is 201±8 Bq/m². The origin of radionuclides is discussed, based mostly on the observed isotopic ratio of Pu. Significant correlations were found between ^239+240Pu, ²⁴¹Am and ¹³⁷Cs. The effective vertical migration rate seems to be in the order of: ⁹⁰Sr≫Pu>Am>Cs.     

Radioactivity of plutonium isotopes, <Superscript>137</Superscript>Cs and their ratio in sediment,seawater and biota from the east coast of Peninsular Malaysia

This study with sampling expeditions of marine sediment, seawater and biota were performed at 30 stations within Malaysian Exclusive Economic Zone (EEZ). A total of >400 samples were collected to determine the activity concentration of anthropogenic radionuclides (^239+240Pu, ¹³⁷Cs) and their activity ratio (^239+240Pu/¹³⁷Cs) in sediments, seawater and biota. The purpose of this study was to determine the concentration levels for these radionuclides and to evaluate any occurrence of radioactive contamination. Sediment cores were obtained using multicorer device, while water samples via co-precipitation techniques and biota was purchased from local fishermen. The activity concentrations of ^239+240Pu in sediment, seawater and biota were ranged 0.21–0.45 Bq/kg dry wt., 2.33–7.95 mBq/m³ and <0.008 Bq/kg fresh wt., respectively. Meanwhile, the values of ¹³⁷Cs were ranged <1.00–2.71 Bq/kg dry wt. in sediment, 3.40–5.89 Bq/m³ in seawater and <0.05–0.41 Bq/kg fresh wt. in biota, respectively. Activity ratios of ^239+240Pu to ¹³⁷Cs obtained seem to confirm that these artificial radioactivities were mainly due to global nuclear fallout.     

Contents of238Pu,239,240Pu and137Cs in sediments and shore depositions of the Vltava river in 1995–1996

The²³⁸Pu,^239,240Pu and¹³⁷Cs concentrations in sediments and shore deposition samples of the Vltava river were determined.^239,240Pu and¹³⁷Cs concentrations in sediment samples (five locations) ranged from 19.6 to 124.8 mBq·kg⁻¹ and from 1.8 to 28.2 Bq·kg⁻¹, respectively. The²³⁸Pu,^239,240Pu and¹³⁷Cs concentrations in shore deposition samples (four locations) ranged from 2 to 16.8, from 26.8 to 477.2 mBq·kg⁻¹, and from 1.6 to 86.3 Bq·kg⁻¹, respectively. The superficial activity of studied radionuclides in shore deposition areas was determined and radionuclide origin at studied locations was discussed.     

Distribution of3H,137Cs and239,240Pu in the surface seawater around Korea

The concentrations of³H,¹³⁷Cs and^239,240Pu were determined in surface seawaters collected at 21 sampling stations around Korea from October of 1994 to May of 1995. The results were consistent with the past data observed in the North Pacific. The concentrations of³H and¹³⁷Cs did not show much difference no matter where the samples were taken. Due to the limited distribution of sampling points, no systematic change in³H and¹³⁷Cs levels with latitude was observed. On the other hand,^239,240Pu concentration in the East Sea (Japan Sea) was somewhat higher than that in the South and the Yellow Seas, although the data on^239,240Pu concentration were not enough to explain the reason. The activity ratios of^239,240Pu/¹³⁷Cs in surface seawater ranged from 0.13% to 0.44% with a mean of 0.25±0.08%. The activity ratios were lower than those of the global fall-out level, 1.1%. This result presumably arose from the different behavior of the two radionuclides in seawater.     

Deposition of90Sr and plutonium isotopes derived from the Chernobyl accident in Japan

To clarify environmental effects of the Chemobyl radionuclides, long-lived Chernobyl radioactivity (^239,240Pu,²³⁸Pu,²⁴¹Pu and⁹⁰Sr) in deposition samples in May 1986 was measured at 11 stations in Japan. Temporal variation of weekly deposition of⁹⁰Sr differed from that of volatile radionuclides such as¹³¹I and¹³⁷Cs, which may reflect the released process at Chernobyl. On the other hand, the geographical distributions of the monthly deposition of long-lived radionuclides were similar to those of volatile radionuclides, in which maximum deposits of⁹⁰Sr and plutonium were observed in Akita, a northwestern Japan Sea coast site of Honshu Island. Higher²⁴¹Pu deposition in most of the stations, as well as high²³⁸Pu/^239,240Pu activity ratios were observed. The²⁴¹Pu/²³⁸Pu activity ratios in deposition samples were nearly equal to that in the total release, which is clear evidence that Chernobyl-derived plutonium was transported to Japan in May 1986 together with volatile radionuclides although the contribution of Chernobyl Pu was about three orders of magnitude lower than¹³⁷Cs.     

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.     

Studies of the vertical distribution of134Cs,137Cs,238Pu,239, 240Pu,241Pu,241Am and210Pb in ombrogenous mires at mid-latitudes

Six peat cores taken from three unmodified blanket and raised bogs in Ireland were sectioned and analyzed for a range of radionuclides including¹³⁴Cs,¹³⁷Cs,²³⁸Pu,²³⁹Pu,²⁴¹Am, and²¹⁰Pb.¹³⁴Cs and¹³⁷Cs were measured by high resolution gamma-spectrometry, while the transuranium nuclides were determined after chemical separation by alpha-spectrometry.²⁴¹Pu, present on the electroplated discs together with Pu(), was measured directly by low-level liquid scintillation counting. Core chronologies were established by measuring the unsupported²¹⁰Pb component using low energy photon spectrometry (LEPS). From the resulting profiles, relaxation depths and migration rates for the above mentioned radionuclides have been determined and differences in the values of these parameters interpreted.²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu ratios have been examined carefully and are discussed in some detail. Finally, the contribution from Chernobyl to the total radiocaesium inventory in each core has been established using the¹³⁴Cs/¹³⁷Cs ratio observed in the initial fallout from Chernobyl.