Plutonium Signatures in a Dated Sediment Core as a Tool to Reveal Nuclear Sources in the Baltic Sea.

Plutonium distribution was studied in an undisturbed sediment core sampled from the Tvären bay in the vicinity of the Studsvik nuclear facility in Sweden. The complete analysis, including minor isotopes, of the Pu isotope composition (238Pu, 239Pu, 240Pu, 241Pu, 242Pu, and 244Pu) allowed us to establish the Pu origin in this area of the Baltic Sea and to reconstruct the Studsvik aquatic release history. The results show highly enriched 239Pu, probably originating from the Swedish nuclear program in the 1960s and 1970s and the handling of high burn-up nuclear fuel in the later years. In addition, the 244Pu/239Pu atomic ratio for the global fallout period between 1958 and 1965 is suggested to be (7.94 ± 0.31)·10-5. In the bottom layer of the sediment, dated 1953-1957, we detected a higher average 244Pu/239Pu ratio of (1.51 ± 0.11)·10-4, indicating the possible impact of the first US thermonuclear tests (1952-1958).

An overview of plutonium isotopes in soils, China: Distribution, spatial patterns, and sources.

Plutonium (Pu) is an anthropogenic radionuclide which has drawn significant attentions due to its radiotoxicity, and the sources of plutonium linked with nuclear accidents and contaminations. The 240Pu/239Pu atom ratio is source dependent and can be used as a fingerprint to determine the sources of radioactive contaminant. However, the distribution and sources of plutonium in soils of China have not yet been systematically studied at a national scale up to date. The distribution, spatial patterns, and sources of plutonium in soils of China were discussed in this work. The concentrations of 239,240Pu are in the range of 0.002-4.824 mBq/g with a large variation, and the 239,240Pu concentrations in surface soils increase with the increasing latitude, which affects by multi-factors such as organic matter and particle size, etc. The inventories of 239,240Pu are in the range of 7.31-554 Bq/m2. The weighted average of 240Pu/239Pu atom ratios (0.180 ± 0.004) in all surface samples is good agreement with the ratio of global fallout (0.180 ± 0.014) of the nuclear weapons tests, this indicate that the major source of plutonium in China is global fallout. However, among some sites, distinctly lower 240Pu/239Pu atom ratio compared to the global fallout values were observed in the northwest China, indicating a significant contribution from other source besides the global fallout. Furthermore, the spatial clustering patterns of hot spots (high values) and cold spots (low values) for plutonium showing the clear associations with nuclear tests, especially the Chinese Lop Nor nuclear weapons tests (CNTs) and the Semipalatinsk nuclear weapons tests (STS). Radioactive material including plutonium from the STS or CNTs was transported by the prevailing westerlies to the northwest China. This review about the fingerprints and distribution of plutonium in soils of China will help researchers to establish a reference database for future radiation risk assessment and environmental radioactive management.

70-Year Anthropogenic Uranium Imprints of Nuclear Activities in Baltic Sea Sediments.

A strongly stratified water structure and a densely populated catchment make the Baltic Sea one of the most polluted seas. Understanding its circulation pattern and time scale is essential to predict the dynamics of hypoxia, eutrophication, and pollutants. Anthropogenic 236U and 233U have been demonstrated as excellent transient tracers in oceanic studies, but unclear input history and inadequate long-term monitoring records limit their application in the Baltic Sea. From two dated Baltic sediment cores, we obtained high-resolution records of anthropogenic uranium imprints originating from three major human nuclear activities throughout the Atomic Era. Using the novel 233U/236U signature, we distinguished and quantified 236U inputs from global fallout (45.4-52.1%), Chernobyl accident (0.3-1.8%), and discharges from civil nuclear industries (46.1-54.3%) to the Baltic Sea. We estimated the total release of 233U (7-15 kg) from the atmospheric nuclear weapon testing and pinpointed the 233U peak signal in the mid-to-late 1950s as a potential time marker for the onset of the Anthropocene Epoch. This work also provides fundamental 236U data on Chernobyl accident and early discharges from civil nuclear facilities, prompting worldwide 233U-236U tracer studies. We anticipate our data to be used in a broader application in model-observation interdisciplinary research on water circulation and pollutant dynamics in the Baltic Sea.

Long-term radiocarbon variation studies in the air and tree rings of Slovakia.

Fifty-five years of radiocarbon variation studies are reviewed with an emphasis on a better understanding of the impacts of the Bohunice nuclear power plant and fossil fuel CO2 on the atmosphere and biosphere of Slovakia. The maximum Δ14C levels in the air up to about 1200‰ were observed during the 1970s at the Zlkovce monitoring station, which after 2005 decreased to <30‰. A relative decrease in the atmospheric Δ14C levels due to increasing levels of fossil CO2 in the atmosphere has also been significant, for example, in Bratislava down to about -330‰, but after 2005 they were only <50‰ below the Jungfraujoch European clean-air level. The tree-ring data, averaging the annual Δ14C levels for several stations in Slovakia, have been in agreement with the atmospheric data, as well as with the newly established clean-air station at Jasná in central Slovakia. Future 14C levels will depend strongly on fossil CO2 levels in the atmosphere, which will change the bomb 14C era to the fossil CO2 era. New investigations of 14C variations in the atmosphere-biosphere-hydrosphere compartments represent a great challenge for radiocarbon science, important for better understanding of environmental processes, climate change, and impacts of human activities on the total environment. This new era of radiocarbon research will also need new developments in radiocarbon analytical technologies, as further progress in accuracy and precision of results (<1‰) will be needed to meet the new radiocarbon challenges.

Spatial distribution, source identification, and transportation paths of plutonium in the Beibu Gulf, South China Sea.

To investigate the spatial distribution and source of plutonium isotopes in the Beibu Gulf, surface sediments were collected and analyzed using sector field inductively coupled plasma mass spectrometry (SF-ICP-MS). The activities of 239+240Pu in surface sediments ranged from 0.012 to 0.451 mBq/g (mean: 0.171 ± 0.138 mBq/g, n = 36), indicating a decreasing trend in a counterclockwise direction from the southern bay mouth. The counterclockwise decreasing trend in the south of the bay mouth is similar to the current in the Beibu Gulf. The 240Pu/239Pu atom ratios in surface sediments ranged from 0.156 to 0.283 (mean: 0.236 ± 0.031, n = 36), slightly higher than that of the global fallout value of 0.18. This suggests that the Pu in the Beibu Gulf was a combination of global fallout and Pacific Proving Ground (PPG). The average contribution of the plutonium (Pu) derived from the PPG in the sediment was estimated to be 52 % ± 24 %.

Review of the sources and behaviors of plutonium isotopes in the atmosphere and ocean.

Plutonium, as well as fission products such as 137Cs, had been released into the earth environment in 1945 after the first atmospheric nuclear explosion of plutonium bomb in the desert of New Mexico (USA, July 16) and later over Nagasaki (August 9), followed then by many other explosions. Thus, plutonium cycling in the atmosphere and ocean has become a major public concern as a result of the radiological and chemical toxicity of plutonium. However, plutonium isotopes and 137Cs are important transient tracers of biogeochemical and physical processes in the environment, respectively. In this review, we show that both physical and chemical approaches are needed to comprehensively understand the behaviors of plutonium in the atmosphere and ocean. In the atmosphere, plutonium and 137Cs attach with aerosols; thus, plutonium moves according to physical and chemical processes in connection with aerosols; however, since plutonium is a chemically reactive element, its behavior in an aqueous environment is more complicated, because biogeochemical regulatory factors, in addition to geophysical regulatory factors, must be considered. Meanwhile, 137Cs is chemically inert in aqueous environments. Therefore, the biogeochemical characteristics of plutonium can be elucidated through a comparison with those of 137Cs, which show conservative properties and moves according to physical processes. Finally, we suggest that monitoring of both plutonium and 137Cs can help elucidate geophysical and biogeochemical changes from climate changes.

Assessment of soil-soil solution distribution coefficients of global fallout 237Np and 239Pu in Japanese upland soils.

Neptunium-237 and 239Pu are important radionuclides in the safety assessment related to geological disposal of radioactive waste because of the possibility of long-term exposure to humans. Mobilities of these radionuclides in the environment are of particular importance for their radiation dose evaluation; therefore, in this study, we have made the assessment of the soil-soil solution distribution coefficient (Kd, L/kg) using global fallout 237Np and 239Pu in Japanese upland soils. The Kd values were determined by extracting these radionuclides from 24 soil samples using a laboratory batch method. The desorption Kd values of 237Np ranged from 3.3 × 102 to 1.0 × 104 L/kg, and their geometric mean (GM) and arithmetic mean (AM) were 1.7 × 103 L/kg and 2.6 × 103 L/kg, respectively. The desorption Kd values of 239Pu were found to vary from 9.4 × 103 to 7.1 × 104 L/kg, and their GM and AM were 3.3 × 104 L/kg and 4.0 × 104 L/kg, respectively. In Japanese upland soils, the Kd value of 239Pu was one order of magnitude higher than that of 237Np.

129I in the SE-Dome ice core, Greenland: A new candidate golden spike for the Anthropocene.

The Anthropocene is a proposed geological epoch that will mark the time when humans have irreversibly affected the Earth. One of the primary requirements to formally establish this is a Global Boundary Stratotype Section and Point or "golden spike" - a record of a planetary signal marking the new epoch's beginning. The leading candidates for the Anthropocene's golden spike are the fallout peaks of 14C (T1/2 = 5730 y) and 239Pu (T1/2 = 24,110 y) from nuclear weapons testing in the 1960s. However, these radionuclides' half-lives may not be long enough for their signals to be observable in the far future and are, thus, not durable. In this regard, here we show the 129I time series record (1957-2007) of the SE-Dome ice core, Greenland. We find that 129I in SE-Dome records almost the entire history of the nuclear age in excellent detail at a time resolution of about four months. More specifically, 129I in SE-Dome reflects signals from nuclear weapons testing in 1958, 1961, and 1962, the Chernobyl Accident in 1986, and various signals from nuclear fuel reprocessing within the same year or a year after. The quantitative relationships between 129I in SE-Dome and these human nuclear activities were established using a numerical model. Similar signals are observed in other records from various environments worldwide, such as sediments, tree rings, and corals. This global ubiquity and synchronicity are comparable to those of the 14C and 239Pu bomb signals, but the much longer half-life of 129I (T1/2 = 15.7 My) makes it a more durable golden spike. For these reasons, the 129I record of the SE-Dome ice core can be considered an excellent candidate for the Anthropocene golden spike.

Transfer of 137Cs and 90Sr from soil-to-potato: Interpretation of the association from global fallout in Aomori to accidental release in Fukushima and Chornobyl.

Ceasium-137 and 90Sr are major artificial radionuclides that have been released into the environment. Soil-to-plant transfer of radionuclides is an important route to food contamination. The radionuclide activity concentrations in crops must be quantitatively predicted for estimating the internal radiation doses from food ingestion. In this study, soil and potato samples were collected from three study sites contaminated with different sources of 137Cs and 90Sr: Aomori Prefecture (global fallout) and two accidental release areas (Fukushima Prefecture and the Chornobyl exclusion zone). The 137Cs activity concentrations in the soil and potato samples widely ranged from 1.0 to 250,000 and from 0.048 to 200,000 Bq kg-1 dry weight, respectively. The soil-to-potato transfer factor of 137Cs also ranged widely (0.0015-1.1) and decreased with increasing concentration of exchangeable K. Meanwhile, the activity concentrations of 90Sr in the soil and potato samples were 0.50-64,000 and 0.027-18,000 Bq kg-1 dry weight respectively, and the soil-to-potato transfer factor of 90Sr was 0.023-0.74, decreasing with increasing concentration of exchangeable Ca. The specific activity ratios of 137Cs/Cs and 90Sr/Sr in the exchangeable fraction were similar to those in potatoes, with a factor of 3 in the ±95 % confidence intervals over six orders of magnitude and a factor of 2 in the ±95 % confidence intervals over five orders of magnitude, respectively. According to the data, the accuracy of predicting the activity concentrations of 137Cs and 90Sr in potatoes can be improved by applying the specific activity ratios of 137Cs/Cs and 90Sr/Sr in the exchangeable fraction. This approach accounts for variable factors such as the effects of K and Ca fertilization and soil characteristics. It also emphasizes the benefit of determining the stable Cs and Sr concentrations in potatoes and other crops prior to possible future contamination.

Plutonium in sediments of the Eastern Guangdong coast-its sources and their contribution.

The 239+240Pu activities and 240Pu/239Pu atom ratios of surface sediments from the Eastern Guangdong coast (EGDC) were determined by sector field ICP-MS in order to examine the sources of plutonium (Pu) and quantify their contributions. The 239+240Pu activities in the EGDC ranged from 0.113 to 0.451 Bq kg-1, with an average of 0.225 ± 0.090 Bq kg-1 (n = 17). Consistently high 240Pu/239Pu atom ratios, ranging from 0.218 to 0.274 (average = 0.254 ± 0.014, n = 17), indicate a non-global fallout Pu source in the EGDC. The horizontal distribution of the 240Pu/239Pu atom ratios in the EGDC sediment suggests the non-global fallout Pu is sourced from close-in fallout from the Pacific Proving Grounds (PPG). Using a simple two end-member mixing model, we calculated the relative proportions of Pu from the PPG and global fallout in the EGDC to be 57 ± 9 % and 43 ± 9 %, respectively. Moreover, from the well-defined relationship between 239+240Pu activity and total organic carbon content in sediments and a two end-member mixing model using δ13C, we further calculated the Terr-global fallout (riverine input) and Mar-global fallout (direct atmospheric deposition) to be 11 ± 2 % and 32 ± 6 %, respectively. Finally, from the activity levels and atom ratios of Pu isotopes in the EGDC, we established a baseline for future use in environmental risk assessment related to nuclear power plant operations.

Simulated inventory and distribution of 137Cs released from multiple sources in the global ocean.

Radioactive cesium (137Cs) is distributed in the world's oceans as a result of global fallout from atmospheric nuclear weapons tests, releases from fuel reprocessing plants, and inputs from nuclear power plant accident. In order to detect future radionuclide contamination, it is necessary to establish a baseline global distribution of radionuclides such as 137Cs and to understand the ocean transport processes that lead to that distribution. In order to aid in the interpretation of the observed database, we have conducted a suite of simulations of the distribution of 137Cs using a global ocean general circulation model (OGCM). Simulated 137Cs radioactivity concentrations agree well with observations, and the results were used to estimate the changes in inventories for each ocean basin. 137Cs activity concentration from atmospheric nuclear weapons tests are expected to be detectable in the world ocean until at least 2030.

Distribution of plutonium isotopes in soils between two nuclear test sites: Semipalatinsk and Lop Nor.

Plutonium (Pu) has attracted attention as an environmental tracer due to its radiotoxicity and the possibility of sources linked with nuclear accidents in recent years. Plutonium isotopes (239,240Pu) were detected at trace levels in soils collected from the Xinjiang region located between the Semipalatinsk nuclear test site and China's Lop Nor nuclear test site. Little is known regarding the spatial variation of 239,240Pu in soils from this region. This study reports the use of Sector Field Inductively Coupled Plasma Mass Spectrometry (SF-ICP-MS) methods to distinguish between Pu isotopes derived from global fallout and nuclear weapon tests. We found that the 239,240Pu activity concentrations ranged from 0.035 to 1.338 mBq/g; the 240Pu/239Pu atomic ratios were 0.157-0.223 with a weighted average of 0.180 ± 0.002, corresponding with the expected average global fallout ratio of 0.180 ± 0.014. This indicated that global fallout is the major source of Pu in the study region. The 239,240Pu inventories in these soils ranged from 23.67 to 222.7 Bq/m2, corresponding with those from other areas in China and other countries within the latitude range. Our Pu isotope data was supplemented with other published Pu data for soils collected in the vicinity of the Semipalatinsk nuclear test site and Lop Nor nuclear test site. Results indicate that 239,240Pu inventories and 240Pu/239Pu atomic ratios in soils exhibit large variations with distance from the Semipalatinsk nuclear test site. High deposition and accumulation of Pu, and low 240Pu/239Pu ratios were observed in close-in fallout and downwind regions of the Semipalatinsk nuclear test site and China's Lop Nor nuclear test site.

Enhancement of Mass Interception Coefficient Data of Radiostrontium by Leafy Crops Using Global Fallout 90Sr and Naturally Occurring 7Be.

When artificial radionuclides are released into the atmospheric environment, one of the important processes by which they affect the human radiation dose is the direct deposition of the radionuclides onto crop surfaces. Because leafy vegetables are consumed while fresh and often raw, the mass interception coefficient [= concentration in food (Bq/kg dry mass (DM) or fresh mass)/total deposition (Bq/m2)] is a key parameter for estimating radionuclide concentrations in crops after the deposition of radionuclides on plant stands. However, such data are still sparse, especially for radiostrontium (89Sr and 90Sr). To enhance the mass interception coefficient data for leafy crops, we used global fallout 90Sr data in leafy crops harvested in 1963-1965 and the deposition data for the corresponding crop growing period. Geometric mean values of the mass interception coefficient of 90Sr for leafy crops were 2.8 m2 kg-1 DM for spinach, 0.60 m2 kg-1 DM for cabbage, and 1.3 m2 kg-1 DM for Chinese cabbage. For comparison, we measured naturally occurring 7Be in giant butterbur leaves, and the results showed that the data were similar to those of 90Sr for spinach. These data were similar to the previously obtained data by single spike radiotracer experiments. Therefore, in the case of nuclear emergency situations, mass interception coefficient data obtained using global fallout 90Sr and/or naturally occurring 7Be should be valuable to estimate radioactivity contamination levels of radiostrontium directly deposited on leafy crops.

Soil-soil solution distribution coefficients of global fallout 239Pu and 237Np in Japanese paddy soils.

239Pu and 237Np are long-lived radionuclides that emit alpha rays, and once released into the environment, they are present there for a long period of time. Therefore,239Pu and 237Np are important radionuclides in the safety assessment related to geological disposal of radioactive waste because of the possibility of long-term exposure to humans. Mobilities of these radionuclides in the environment are of particular interest; therefore, in this study, we have made the first-time determination of the soil-soil solution distribution coefficient (Kd, L/kg) using global fallout 239Pu and 237Np in soil. The Kd values were determined by extracting these radionuclides from 23 soil samples using a laboratory batch method. The desorption Kd values of 239Pu were found to vary from 3.2 × 103 to 1.4 × 105 L/kg, and their geometric mean (GM) and arithmetic mean (AM) were 2.3 × 104 L/kg and 3.2 × 104 L/kg, respectively. The desorption Kd values of 237Np ranged from 8.9 × 102 to 2.1 × 104 L/kg, and their GM and AM were 4.1 × 103 L/kg and 6.4 × 103 L/kg, respectively. A comparison between the obtained Kd values of 239Pu and 237Np indicated that the former were about 6-fold higher than the latter in Japanese paddy field soils. Pearson's correlation analysis suggested that the main factors contributing to the sorption and desorption of Pu isotopes in Japanese paddy soils were related to the amounts of Fe and Mn oxides, while the sorption and desorption of 237Np in them would be controlled by an ion-exchange reaction, and/or complex-formation with organic matter, especially in Fluvisols.

Estimation of radionuclides global fallout levels in the soils of CIS and eastern Europe territory.

This study is devoted to the estimation of radionuclides global fallout levels in the soils of Commonwealth of Independent States (CIS) and Eastern Europe territory as a result of nuclear explosions. 58 standard soil samples were used, which were selected in different soil and climatic areas of the territory of CIS and Eastern Europe in 1978-2018. All samples were measured by gamma spectrometry. Determination of plutonium isotopes and strontium was performed according to the method of the joint determination of these radionuclides from one sample. IN the samples considered in this work, the content of 60Co, 154Eu, 155Eu was below the detection limits, which were 0.4; 1.0 and 1.0, respectively. Natural radionuclides analysis results indicated that the obtained samples are typical soil samples without its abnormal contents. The content of 137Cs, 90Sr, 239+240Pu in a 20 cm soil layer due to global fallout is (3.9 ± 1.7), (2.2 ± 0.8), (0.18 ± 0.08) Bq/kg respectively, which considering the distribution of these radionuclides by depth and average soil density is (1.2 ± 0.5) kBq/m2 for 137Cs, (0.42 ± 0.15) kBq/m2- 90Sr and (55.0 ± 24.0) Bq/m2- 239+240Pu. The isotopic ratios137Cs/90Sr and 137Cs/239+240Pu for the territory of CIS and Eastern Europe are at the level (2.0 ± 0.71) and (25 ± 15), respectively.

Deciphering anthropogenic uranium sources in the equatorial northwest Pacific margin.

This work reports the first high-resolution deposition records of anthropogenic uranium (236U and 233U) in a sediment core taken at the continental slope of the Philippine Sea off Mindanao Island in the equatorial northwest Pacific Ocean. Two notable peaks were observed in both profiles of 236U and 233U concentrations, with a narrower peak in 1951-1957 corresponding to close-in Pacific Proving Grounds (PPG) signal, and a broader peak in 1960s-1980s corresponding to the global fallout from nuclear weapons testing. 236U and 233U areal cumulative inventories in the studied sediment core are (2.79 ± 0.20) ∙ 1012 atom ∙ m-2 and (3.12 ± 0.41) ∙ 1010 atom ∙ m-2, respectively, about 20-30% of reported 233U and 236U inventories from the direct global fallout deposition. The overall 233U/236U atomic ratios obtained in this work vary within (0.3-3.5) âˆ™ 10-2, with an integrated 233U/236U atomic ratio of (1.12 ± 0.17) âˆ™ 10-2. The contribution from global fallout and close-in PPG fallout to 236U in the sediment core is estimated to be about 69% and 31%, respectively. We believe the main driving process for anthropogenic uranium deposition in the Philippine sediment is continuous scavenging of dissolved 236U from the surface seawater by sinking particles.

Distributions of fallout 137Cs, 239+240Pu and 241Am in a soil core from South Central China.

The source and vertical distribution of 137Cs,239+240Pu and 241Am activity concentrations in a soil core from Hunan Province, China were investigated. The maximum 137Cs and 239+240Pu activity concentrations were 15.45 ± 0.76 mBq/g and 0.819 ± 0.066 mBq/g, respectively. While the maximum 241Am activity concentration in samples obtained from the core was 0.341 ± 0.019 mBq/g. The 240Pu/239Pu atom ratio and the 137Cs/239+240Pu activity ratio were 0.183 ± 0.011 and 19.5 ± 1.8, respectively, and both were consistent with the characteristic value of global fallout. The integrated 241Am/239+240Pu activity ratio for global fallout was also re-estimated. The measured 241Am/239+240Pu activity ratio (average 0.43 ± 0.07) in the samples was very close to the estimated value (0.45), which suggested their 241Am also came from the global fallout. Regarding the vertical distribution of 137Cs, 239+240Pu and 241Am in these red soil samples, all these radionuclides had higher concentrations in upper layers of several centimeters of soil while they had slightly lower concentrations in lower soil layers down to 30 cm. Vertical distributions of 137Cs/239+240Pu and 241Am/239+240Pu activity ratios indicated the migration velocity was Am ≈ Pu > Cs. The intrinsic chemical properties of the radionuclides as well as soil type and properties (acidic, nutrient-deficient and low in organic matter and cation exchange capacity) might be reasons for the differences in their migration behaviors.

Distributions and impacts of plutonium in the environment originating from the Fukushima Daiichi Nuclear Power Plant accident: An overview of a decade of studies.

This paper reviews the current knowledge on plutonium (Pu) isotopic composition (the atom or activity ratios) and activity concentrations of 238Pu, 239Pu, 240Pu, and 241Pu resulting from the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident in 2011. In this critical review, we document the characteristic values of Pu atom or activity ratios (fingerprints) and present their spatial distributions around the FDNPP site. Based on multiple Pu fingerprints (238Pu/239+240Pu activity ratio, 240Pu/239Pu atom ratio, and 241Pu/239Pu atom ratio), we clarify that Pu contamination from the FDNPP accident occurred in a restricted terrestrial area, while Pu in the Northwest Pacific Ocean is still predominately sourced from the Pacific Proving Grounds (PPG) and global fallout. Using a simple two end-member mixing model, we calculate average contributions of Pu from the FDNPP accident of 13 ± 20% (n = 180) in soil samples, 55 ± 32% (n = 38) in leaf litter samples, and 67 ± 26% (n = 129) in air dust/black substances. In the marine environment, the PPG source average contributions are 45 ± 15% (n = 76) in seawater and 42 ± 12% (n = 48) in sediments. The spatial distributions of Pu atom or activity ratios based on existing studies suggest that: 1) in the terrestrial region investigated 80 km northwest of the FDNPP site, the Pu contamination is mainly observed in an area within a 50 km distance, and 2) in the terrestrial region investigated 60 km southwest of the FDNPP site, the Pu contamination is mainly observed in an area within a 30 km distance. Studies of Cs-bearing radioactive particles indicate that Pu occurs as Pu oxide, and the fuel fragments containing Pu that were released from the reactors to the surrounding environment are associated with micron-scale Cs-bearing radioactive particles. We note that the fractionation between Pu and other radionuclides occurred after release. These new findings about the Pu fingerprints around the FDNPP site will help researchers to establish a reference background database for future environmental risk assessment and geochemical study there.

Temporal change of 236U/238U and 235U/238U isotopic ratios in atmospheric deposition in Tokyo and Akita from 1963 to 1979.

We examine the temporal changes of 236U/238U and 235U/238U in atmospheric deposition from samples collected in Tokyo and Akita from 1963 to 1979 and elucidate the spatial distribution and historical changes of the anthropogenic sources of uranium in Japan. The 236U/238U ratio of atmospheric deposition in Tokyo peaked in 1963 and again during the 1970s, while the corresponding 235U/238U ratios of atmospheric deposition during the second peak period were lower than that of natural uranium. The 236U/238U ratios of atmospheric deposition in Akita samples peaked in 1963. The 235U/238U ratios in Akita samples were almost identical to that of the natural uranium ratios. These results suggest that the peak of 236U/238U in 1963 corresponds to what is recognized as representative for global fallout. The increase of 236U/238U and the decrease of 235U/238U observed simultaneously in the 1970s indicate that depleted uranium has subsequently been released into the environment around Tokyo. The cumulative deposition density of 236U for atmospheric fallout samples collected in Tokyo from 1968 to 1979 is an order of magnitude larger than that of the global fallout, suggesting that the depleted uranium in the 1970s is a major component of 236U in Tokyo and should be considered as an end-member when using 236U as an environmental tracer in the industrial city. This knowledge can facilitate future research using 236U as an effective environmental tracer.

Distribution and source of plutonium in sediments from the southern Gulf of Mexico.

Here, we report on new data (75 analyses) of plutonium (Pu) isotopes to elucidate activity concentrations, inventories, sources, and their transport from the ocean surface to the seafloor from a collection of six deep-sea sediment cores (depths ranging from 257 to 3739 m) in the southern Gulf of Mexico. Sediment cores collected from the continental shelf and upper slope region of the Gulf of Mexico showed 240Pu/239Pu ratios of 0.15 to 0.26, and 239+240Pu-inventories ranging from 14.7 to 33.0 Bq m-2. Inventories and ratios are consistent with global fallout Pu for this tropical region. In contrast, sediment cores collected from the lower slope region and abyssal plain showed low 240Pu/239Pu ratios of 0.07 to 0.13 and much lower 239+240Pu inventories below 6.8 Bq m-2. This implies that only a small fraction of the expected global fallout Pu has reached the deep-sea sediments. The low 240Pu/239Pu isotope ratios indicate that fallout from the Nevada testing site was an important source of Pu in deep-sea sediments, and that this Pu was likely more efficiently scavenged from the water column than Pu from global fallout. We estimated that up to 44% of the total inventory of 239+240Pu in deep-sea sediments is due to the Nevada source. Low values and a progressive decrease of 240Pu/239Pu ratios and 239+240Pu inventories with increasing water depth have been previously reported for the Gulf of Mexico. Analysis of Pu isotopes in two sediment traps from the upper slope regions shows 240Pu/239Pu ratios comparable to those observed in global fallout. These results indicate that global fallout Pu is currently the main source of Pu in sinking particles in the water column. Therefore, a significant fraction of global fallout Pu must still be present, either in a dissolved phase, or as biologically recycled material in the water column, or scavenged on the shelf and shelf break. Our results bring to light important questions on the application of Pu isotopes to establish sediment chronologies in deep-sea sediments, since global fallout features such as the 1963 maximum are not available.