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 %.

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.

Temporal evolution of plutonium concentrations and isotopic ratios in the Ukedo - Takase Rivers draining the Difficult-To-Return zone in Fukushima, Japan (2013-2020).

In 2011, the Fukushima Dai-Ichi Nuclear Power Plant (FDNPP) accident released significant quantities of radionuclides into the environment. Japanese authorities decided to progressively reopen the Difficult-To-Return Zone after the decontamination of priority reconstruction zones. These areas include parts of the initially highly contaminated municipalities located to the north of the FDNPP, including Namie Town, an area drained by the Ukedo and Takase Rivers. Eleven years after the accident, research focused on the spatial distribution of plutonium (Pu) and radiocesium (Cs) isotopes at contrasted individual locations. To complement previous results, the current research was conducted on flood sediment deposits collected at the same locations after major flooding events during eleven fieldwork campaigns organised between 2013 and 2020 at the outlet of the Ukedo and Takase Rivers (n = 22). The results highlighted a global decrease of the Pu and 137Cs contents in sediment with time during the abandonment phase in the region, from 2013 (238.20 fg g-1) to 2020 (4.28 fg g-1). Furthermore, based on the analysis of the 240Pu/239Pu isotopic ratios, the plutonium transiting these rivers (range: 0.166 - 0.220) essentially originated from the global fallout (0.180 ± 0.014 (Kelley et al., 1999)). Sediment showed contrasted properties in the two investigated rivers, which is likely mainly the result of the occurrence of Ogaki Dam on upper sections of the Ukedo River as it strongly impacts the material supply from this river to the Pacific Ocean. A statistical analysis highlighted the strong correlation between Pu activity concentrations and 137Cs activities in both rivers, confirming that both radionuclides are transported with a similar pathway. Despite it was detected early after the accident (2011-2013), the current research demonstrates that plutonium originating from FDNPP is no longer detected in these rivers draining the Difficult-To-Return Zone at the onset of the reopening of the area to its former inhabitants.

Retrospective determination of fallout radionuclides and 236U/238U, 233U/236U and 240Pu/239Pu atom ratios on air filters from Vienna and Salzburg, Austria.

137Cs and 241Pu (via 241Am) concentrations were measured γ-spectrometrically on air filters from the early 1960s (mainly from 1964-66) from Vienna, Austria, and an alpine station in Salzburg, Austria. Accelerator mass spectrometry (AMS) was used to determine 240Pu/239Pu, 236U/238U and 233U/236U atom ratios as well as 236U, 239Pu and 240Pu atom concentrations. The maximum 236U/238U atom ratio of these unique undisturbed global fallout samples was (1.19 ± 0.31) × 10-5 in spring 1964. The 233U/236U atom ratios were found within (0.15-0.49) × 10-2 and indicate that the weapons tests of the early 1960s can be excluded as 233U source. The 236U/239Pu atom ratios were calculated in the range of 0.22-0.48.

Spatio-temporal distribution of 239+240Pu in sediments of the China sea and adjacent waters.

Data of 239+240Pu activities and 240Pu/239Pu atom ratios in surface and core sediments of the China Sea and adjacent waters were collected. We examine a dataset of 239+240Pu activities and 240Pu/239Pu ratios determined from surface sediments at 516 sites and 84 core sediment mainly across the China Sea and adjacent waters. For the first time the spatial distributions of the 239+240Pu activities, the 240Pu/239Pu ratios and the Pacific Proving Ground (PPG) fraction in the China Sea and adjacent waters are fully presented at the same time. Four types of typical 239+240Pu distribution with depth are commonly summarized: non-peak, pseudo single peak, single peak and multi peaks, which are based on the comprehensive analysis of the vertical distribution of 239+240Pu in 84 sediment cores that had been studied in the China Sea and adjacent waters. Their occurrence probability are ∼15%, ∼4%, ∼67% and ∼11%, respectively. This is the dominant Pu source in seawater which was transported by the North Equatorial Current and Kuroshio Current and its extension into the China Sea and adjacent waters first from east to west, then from south to north. A sea area to the northeast of Taiwan Island and the Okinawa Trough, shows high 239+240Pu activities and 240Pu/239Pu atom ratios spatial distribution trends, which are related to the intrusion of the Kuroshio Current carrying 239+240Pu from the PPG nuclear weapon tests. The used two end-member mixing model suggests that global fallout and PPG close-in fallout are the main sources of Pu in most of the investigate areas. As the 240Pu/239Pu of global fallout is relatively constant, the change of 240Pu/239Pu ratios in surface sediments of the China Sea and adjacent waters are mainly controlled by the PPG close-in fallout input.

Retrospective determination of U and Pu isotopes and atom ratios in lung samples from Vienna, Austria.

Uranium and plutonium isotope concentrations as well as 236U/238U and 240Pu/239Pu atom ratios were measured by AMS in human lung samples from the early 1960s. The 236U concentrations as well as the 236U/238U atom ratios show a maximum in 1964, 239Pu and 240Pu concentrations are increasing continually from 1962 to 1965. 236U/238U atom ratios are lower by two orders of magnitude compared to corresponding aerosol data from Vienna, probably due to older 238U deposited in the lungs, enhanced 238U concentrations in the city air, and activity partition within different particle sizes. The 236U/239Pu atom ratios in lung samples are also lower than expected from the aerosol data, while 240Pu/239Pu atom ratios lie well within the range typical for nuclear bomb fallout.

Spatial distribution and migration of 239+240Pu in Chinese soils.

The migration of radionuclides is a critical threat to the soil and groundwater environment. This study investigates highly radiological toxic 239+240Pu in 647 surface soils and 66 soil cores in China. First, the spatial distributions of 239+240Pu activities and 240Pu/239Pu ratios are presented in Chinese surface soils. Second, four different types of vertical distribution of 239+240Pu, namely 45.4%, 40.9%, 9.1% and 4.5% of Chinese soil cores proportions are integrated using statistical analysis. Furthermore, different soil types are accompanied by different 239+240Pu vertical distributions, which relate closely to the 239+240Pu migration. Finally, based on the Convection Dispersion Equation (CDE) model, the present work find that the apparent convection velocities of 239+240Pu are ranging from 0.00032 ± 0.00031 cm a-1 to 0.473 ± 0.083 cm a-1. As shown by the four typical vertical activity distribution of 239+240Pu in soil cores, the deepened activity maximum value position of 239+240Pu implies a fast migration rate or apparent convection velocity. This study, for the first time, suggests a significant linear correlation (R2 = 0.847) between the depth of 239+240Pu maximum value (cm) and the apparent convection velocity (v, cm a-1). We hypothesize that v usually does not exceed 0.5 cm a-1 in the CDE model. A significant linear correlation is also identified between apparent dispersion coefficient (D, cm2 a-1) and v2 in Chinese soil cores from the CDE model. It will provide an important reference for harmful heavy metal migration research in the future.

Plutonium isotopes in the northwestern South China Sea: Level, distribution, source and deposition.

The spatial distribution of plutonium isotopes (239Pu, 240Pu) in the surface sediments collected from the northwestern South China Sea (SCS) in 2018 was investigated. The 239,240Pu concentrations in surface sediments vary from 0.048 to 0.960 mBq/g (with mean of 0.282 ± 0.242 mBq/g) depending on the geographical feature of the sampling location such as the river estuary, continental shelf, slope and deep basin. Higher 240Pu/239Pu atomic ratios (0.24-0.31) in the surface sediment of the SCS compared to the global fallout value of 0.18 were observed, this is attributed to the input of close-in fallout of the Pacific Proving Ground (PPG) transported by the North Equatorial Current and Kuroshio Current to the northern SCS. The contribution of the PPG derived plutonium in the SCS sediment was estimated to be 39%-78% using a simple two-end member mixing model based on the measured 240Pu/239Pu atomic ratios in the sediment. Besides the soluble 239,240Pu level in seawater, load of suspended particulate matter from the river runoff and biological debris, hydrographic and hydrodynamic conditions are key parameters influencing the deposition process of plutonium to the sediment.

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.

Temporal trend of 240Pu/239Pu atom ratios in water columns in the Western North Pacific Ocean and its marginal seas.

The 240Pu/239Pu atom ratios were determined by inductively coupled plasma mass spectrometry for seawater samples from the Okinawa Trough in the western North Pacific Ocean margin to identify their Pu sources and to elucidate the temporal variability in atom ratios in the water columns in the western North Pacific Ocean and its marginal seas. The 239Pu, 240Pu and 239+240Pu water column inventories were 12.2 ± 0.5, 10.5 ± 0.5 and 22.7 ± 0.7 Bq m-2, respectively. The observed 240Pu/239Pu ratios were clearly greater than the mean global fallout ratio of ∼0.18 with a mean value of 0.236 ± 0.014. The observed greater atom ratios confirmed the presence of close-in fallout Pu from nuclear testing at the Pacific Proving Grounds (PPG). The relative percentage of the PPG-derived Pu to global fallout Pu was estimated as 41 ± 10%. The 239+240Pu water column inventory originating from the PPG close-in fallout was also calculated as 9.2 ± 0.4 Bq m-2. The temporal variability in the mean 240Pu/239Pu atom ratios in the water columns in the western North Pacific Ocean and its marginal seas was obtained through comparison of the present study values and the previously reported values, and it had no significant temporal variation with a mean value of 0.237 ± 0.004 during the observation period of 1984-2015. The 239Pu and 240Pu derived from the two different sources of global fallout and the close-in fallout at the PPG were homogenized in the water masses in the studied areas.

Assessment of residual radionuclide levels at the Bokak and Bikar Atolls in the northern Marshall Islands.

The Bikar and Bokak Atolls, located in the northern Marshall Islands, are extremely isolated and consist of pristine marine and terrestrial ecosystems. Both atolls may have experienced significant radioactive deposition following the nuclear weapon testing conducted at Bikini and Enewetak proving grounds. Here we report activity concentrations of artificial radionuclides (239Pu, 240Pu, 241Pu, 241Am, 137Cs and 90Sr) in marine and terrestrial samples collected from Bikar and Bokak Atolls. Artificial radionuclides in soil from the Majuro Atoll are also reported and form a radiological baseline against which the levels at the other atolls can be compared. We observed low levels of artificial radionuclides in soil from Majuro and Bokak, but significantly higher levels in soil from Bikar. The residual radioactivity in the Bikar environment is comparable to the levels previously reported for other nearby atolls, including Taka and Utrik, but lower than for Rongerik, Rongelap, Bikini and Enewetak. An analysis of 240Pu/239Pu isotope ratios and estimations of the dates of contamination from 241Am/241Pu activity ratios both indicated that the Bikar Atoll was contaminated mainly by radioactive fallout from the Castle Bravo test in 1954. We compare the results of our measurements at Bikar and Bokak to data from other atolls in the Marshall Islands and to regions of the world affected by both global and regional fallout from atmospheric nuclear weapons testing and nuclear accidents.

Plutonium isotopes and radionuclides in corals around Weizhou land in Beibu Gulf, China.

Plutonium isotopes in the coral were determined with chemical separation method using AG 1-X8 and AG-MP-1M anion exchange resins and sector field inductively coupled plasma mass spectrometry (SF-ICP-MS) in order to elucidate the activity concentration and source of Pu around Weizhou land in Beibu Gulf, China. Furthermore, the activity concentrations of other radionuclides (238U, 226Ra, 232Th, 137Cs, 40K and 210Pb) were measured by a HPGe spectrometer. The activity concentration of 240+239Pu in the coral is determined to be in the range of 8.95-27.84 mBq/kg. The 240Pu/239Pu atom ratios in the samples range from 0.173 to 0.225, indicating that the main source of plutonium in this area is global fallout while the contribution of PPG is about 30%. Further, the activity concentrations of 238U, 232Th, 40K and 226Ra are determined to be in the range of 18.72-64.63, 1.37-20.8, 29.78-72.52 and 3.48-61.97 Bq/kg, respectively.

Distribution of Pu isotopes and 210Pb in the Bohai Sea and Yellow Sea: Implications for provenance and transportation.

Particle-reactive radionuclides are useful for tracing sediment dynamics in marginal seas. We collected a suite of surface sediment samples in May 2014 from the Bohai Sea (BS) and Northern Yellow Sea (NYS) to observe the spatial distribution of Plutonium (Pu) isotopes and 210Pb activities. 239+240Pu activities ranged from 0.001 to 0.288 and 0.040-0.269 Bq kg-1 in BS and NYS surface sediments, respectively. 210Pbex shows a significant correlation with 239+240Pu (r = 0.84, p < 0.01) that suggested these two nuclides were scavenged to the same grade. 240Pu/239Pu atom ratios in BS (0.173-0.256) and NYS (0.196-0.275) were slightly higher than the global fallout value of 0.18 and lower than the Pacific Proving Ground (PPG) value of 0.36, indicating that some fraction of Pu originating from the PPG was capable of being transported to the BS and NYS. Mass balance results showed that 41% of 239+240Pu (8.9 × 109 Bq yr-1) and 18% of 210Pb (2.4 × 1012 Bq yr-1) in the NYS originated in the oceanic input. In the BS, 63% of 210Pb originated from atmospheric deposition and 84% of 239+240Pu originated from riverine input. Using Pu and 210Pb as tracers, we estimate that (1.8-2.6) × 108 t yr-1 and (3.6-3.8) × 108 t yr-1 of sedimentary particles could be transported from the BS to the NYS and from the NYS to the Southern Yellow Sea, respectively. Furthermore, the 226Ra/238U activity ratio distribution suggested that sedimentary particles derived from the Yellow River could be transported to the middle of the BS and coastal areas of the NYS.

Plutonium in Southern Yellow Sea sediments and its implications for the quantification of oceanic-derived mercury and zinc.

The spatial distributions of mercury (Hg) and zinc (Zn) concentration and the isotopic composition of plutonium (Pu) were investigated in surface sediments and sediment cores collected from the Southern Yellow Sea (SYS) during May 2014. The variation of the 240Pu/239Pu atom ratio (0.18-0.31) in the surface sediments of the SYS clearly indicated a signal of close-in fallout input from the Pacific Proving Ground (PPG). The buried 239+240Pu in the sediment of the SYS was estimated to be (4.7 ± 0.5) × 1010 Bq y-1 during the period from 2011 to 2014, of which ∼33% (1.5 × 1010 Bq y-1) was derived from the PPG by long-range transport via ocean currents (e.g., the North Equatorial Current and Kuroshio Current). The concentrations of Hg and Zn varied from 0.003 to 0.067 mg kg-1 and from 43.9 to 137 mg kg-1, respectively, and exhibited positive correlations with the 239+240Pu activity both in the surface sediments (0-1 cm) and upper layers (7 cm) of the sediment cores. Therefore, by using Pu as a tracer, we estimated that the oceanic input contributed 2.0 tons y-1 of Hg and 1.0 × 103 tons y-1 of Zn to the SYS sediments between 2011 and 2014, which accounted for 33% and 3% of total buried Hg and Zn, respectively. These findings indicate that environmental pollution control should also consider the oceanic contribution of some pollutants. The results of the present work help to elucidate the biogeochemical cycling of trace metals in marginal seas, and are helpful for managing environmental pollution in marine environments.

Radionuclides in the environment around the uranium mines in Guangxi, China.

Uranium and plutonium are both poisonous radioactive elements, which are very harmful to human health and environment. Therefore, it is of great significance to study the distribution of 238U concentration and 239+240Pu activity in the uranium mine surrounding soils. We have collected some surface soil sediments within 2 km of two uranium mines and a solid waste management center in Guangxi Province. The 238U concentration in these study areas is in the range of 1.44-83.91 mg/g, and the 238U concentration in the A uranium mine surrounding surface soils is higher than that in the B uranium mine and the solid waste management center. While the B uranium mine and the solid waster management center don't pollute the surrounding soils because the 238U concentrations in their surrounding soils are similar to the average 238U concentration in the soil. The 239+240Pu activities in soil samples collected around the two uranium mines and the solid waste management center are close ranged from 0.06 mBq/g to 0.51 mBq/g. Moreover, the 240Pu/239Pu atom ratios in our study samples are ranged from 0.15 to 0.23, which indicate the Pu may come from the global fallout. In addition, we study heavy metals in our collected samples, only heavy metal Tl has weak positive correlations with 238U concentrations and 239+240Pu activities. And there is a weak positive correlation between 238U concentrations and 239+240Pu activities.

An overview of current knowledge concerning the inventory and sources of plutonium in the China Seas.

This study reviews the current understanding of the inventory and sources of plutonium (Pu) in the marine environment adjacent to China. The 239+240Pu inventory in the China Seas was found to have large spatial variations. The quantity in sediments decreases away from the shore, generally tracing the sedimentation rate distribution. High 239+240Pu inventories indicated that Pu in the water column was easily scavenged since Pu has a high particle affinity. Indeed, substantially higher 240Pu/239Pu atom ratios were observed in the sediment and seawater of the China Seas than are found in global fallout. We thus clarified that Pu sources in the China Seas were from both global fallout and the Pacific Proving Grounds (PPG) in the Pacific Marshall Islands. Plutonium from the latter source is transported into the China Seas through the North Equatorial Current (NEC) and Kuroshio. Using a two end-member mixing model, we revealed that the contribution of Pu from the PPG accounts for over 40% of the Pu in the East China Sea (ECS) and South China Sea (SCS), and less than 20% of the Pu in the Yellow Sea (YS). The distributions and isotopic composition of Pu in the China Seas indicate strong scavenging of Pu in the ECS and high Pu accumulation in the SCS. This information on the inventory and isotopic composition of Pu helps to establish a background for the future study of Pu in the China Seas.

The 240Pu/239Pu atom ratio in Chinese soils.

The 240Pu/239Pu atom ratio is a very effective tool for the identification of the origin of plutonium (Pu) in the soil environment. We examine a dataset of 240Pu/239Pu atom ratios determined from surface and core soils at 240 sites across China. The data were compiled from 18 separate literature sources from the last 20 years. For the first time the spatial distribution (3 latitude bands and 7 natural regions) of the weighted average 240Pu/239Pu atom ratios in Chinese soils is investigated. An area to the West of Xining City, shows a weighted average 240Pu/239Pu atom ratio of 0.167 ±â€¯0.002, lower than that of average global fallout, which likely arises from the addition of local fallout radionuclides from the Chinese nuclear weapon tests at Lop Nor between 1964 and 1980. The Yumen and Jiuquan areas of Northwest China in particular show evidence of very low ratio material from the Chinese nuclear weapon tests. Excluding the impacted area around the test site the weighted average 240Pu/239Pu ratio of 0.182 ±â€¯0.002 suggests that global fallout is the main source of Pu in most Chinese soils.

Anthropogenic 236U and Pu at remote sites of the South Pacific.

Anthropogenic radionuclides, like 236U and 239,240Pu, are present in the environment as a result of global fallout from nuclear weapons tests conducted in the 1950s and 1960s and can potentially be used as tracers in soil erosion and sediment movement studies. Here, we report data on 236U and 239,240Pu in soil samples from the Motueka Valley (New Zealand) and for the first time from two remote islands Rarotonga and Atiu (Cook Islands) in the South Pacific. 236U and 239,240Pu were measured using Accelerator Mass Spectrometry (AMS) at the Australian National University. The 236U and 239Pu isotope concentrations versus soil depth and the 240Pu/239Pu and 236U/239Pu isotope ratios are discussed for each site. The radionuclide depth dependence revealed any soil disturbance, whereas the isotopic signatures indicated the source of the radionuclides' origin.

Pu isotopes in the seawater off Fukushima Daiichi Nuclear Power Plant site within two months after the severe nuclear accident.

The marine environment is complex, and it is desirable to have measurements for seawater samples collected at the early stage after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident to determine the impact of Fukushima-derived radionuclides on this environment. Here Pu isotopes in seawater collected 33-163 km from the FDNPP site at the very early stage after the accident were determined (May 2011, within two months after the accident). The distribution and temporal variation of 239Pu and 240Pu were studied. The results indicated that both 239+240Pu activity concentrations (from 0.81 ±â€¯0.16 to 11.18 ±â€¯1.28 mBq/m3) and 240Pu/239Pu atom ratios (from 0.216 ±â€¯0.032 to 0.308 ±â€¯0.036) in these seawater samples were within the corresponding background ranges before the accident, and this suggested that Fukushima-derived Pu isotopes, if any, were in too limited amount to be distinguished from the background level in the seawater. The analysis of Pu isotopic composition indicated that the major sources of Pu in the seawater after the accident were still global fallout and the Pacific Proving Ground close-in fallout. The contribution analysis showed that the contributions of the Pacific Proving Ground close-in fallout in the water column of the study area ranged from 26% to 77% with the average being 48%.

Sources and scavenging of plutonium in the East China Sea.

The 240Pu/239Pu atom ratio and 239+240Pu activity of seawater in the East China Sea (ECS) was measured in order to examine the Pu sources and elaborate Pu scavenging process. High 240Pu/239Pu atom ratios (0.187-0.243, average = 0.221 ±â€¯0.017) in the surface water and water column were observed during 2011, implying of non-global fallout Pu sources. The distribution of 240Pu/239Pu atom ratio in the ECS was in agreement with the introduction pathway of the Kuroshio, showing a decreasing trend away from the outer shelf. An even higher 240Pu/239Pu atom ratios (0.243-0.263, average = 0.253 ±â€¯0.007) were observed in the Kuroshio, indicating the non-global fallout Pu signal from the Pacific Proving Grounds (PPG). Using a two end-member mixing model, the Pu source from the PPG contribution was calculated to be 36 ±â€¯9% in the ECS seawater. The 239+240Pu activities of surface seawater were in the range of 2.00-2.95 mBq m-3 in the ECS. The spatial distribution of 239+240Pu activity in the surface seawater showed an increasing trend from the outer shelf to the nearshore. Moreover, 239+240Pu inventory of water column at the station DH23 in the ECS was calculated to be ~0.29 Bq m-2, which was 1-3 orders of magnitude lower than the estimates of sediment cores in the ECS shelf (9-407 Bq m-2). Such differences were determined by the high degree Pu scavenging efficiency in the ECS and high Pu input carried by terrestrial sediments from the Yangtze River. Finally, both 240Pu/239Pu atom ratios and 239+240Pu activities were identical before and after the Fukushima nuclear accident (FNA), suggesting that the impact of the FNA on the ECS was negligible.