Pacific Proving Grounds Close-in Fallout Research Articles

Biomonitoring of Pu isotopes in liver of North Pacific giant octopus (Enteroctopus dofleini) collected off the Rokkasho Nuclear Fuel Reprocessing Plant, western North Pacific margin

Concentrations of 239+240Pu and 240Pu/239Pu atom ratios were determined in liver samples of North Pacific giant octopus (Enteroctopus dofleini) collected off the Rokkasho Nuclear Fuel Reprocessing Plant (RNFRP) to understand the bioaccumulation of Pu in the octopus liver, to provide Pu data before full commercial operation of the reprocessing plant, and to identify the sources of Pu isotopes in the studied liver samples. Mean 239+240Pu concentration was 6.3 ± 3.1 mBq/kg-wet, which was within the previously reported concentration ranges in liver of the Japanese common squid and in hepatopancreas of red queen and snow crabs. The 240Pu/239Pu atom ratios ranged from 0.223 to 0.252 with a mean ratio of 0.234 ± 0.009, which was noticeably greater than the mean global fallout ratio of ~0.18. These ratios reflected a mixture of global fallout Pu from atmospheric nuclear weapons testing and close-in fallout Pu from the Pacific Proving Grounds (PPG). The relative percentage of the PPG close-in fallout Pu to global fallout was calculated to be 39.6 ± 6.7%. The liver of the NPG octopus is an excellent bioindicator for biomonitoring of Pu pollution. Data on 239+240Pu concentrations and 240Pu/239Pu atom ratios in liver of the NPG octopus collected in the vicinity of the RNFRP will provide powerful keys for continuous biomonitoring of Pu pollution and for distinguishing the potential sources of Pu after the plant begins full commercial operation.

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.

Transuranic nuclides Pu, Am and Cm isotopes, and 90Sr in seafloor sediments off the Fukushima Daiichi Nuclear Power Plant during the period from 2012 to 2019

The 238Pu, 239+240Pu, 241Am, 242Cm, 243+244Cm and 90Sr concentrations in seafloor surface sediments collected at three sampling stations off the Fukushima Daiichi Nuclear Power Plant (FDNPP) site during the period from 2012 to 2019 were determined to elucidate the impacts of the FDNPP accident onto their concentrations in coastal sediments and to discuss the sources of the measured radionuclides. The 239+240Pu, 241Pu and 241Am concentrations and 240Pu/239Pu atom ratios in a sediment core were also determined to allow comparison of their inventories between this study and previously reported values and to identify the Pu sources. The 238Pu, 239+240Pu, 241Am and 90Sr concentrations showed no remarkable temporal variations; no significant increases in concentrations after the FDNPP accident were observed; these concentrations were comfortably within the previously reported concentration range; and no detectable 242Cm and 243+244Cm amounts were observed in surface sediments. The observed 238Pu/239+240Pu activity ratios were approximately two orders of magnitudes lower than those for the damaged FDNPP reactor core inventories and the observed values in terrestrial samples after the accident. The 239+240Pu, 241Pu and 241Am inventories in the sediment core were 389 ± 5, 503 ± 33 and 214 ± 3 Bq m−2, respectively. The 239+240Pu inventory was about an order of magnitude greater than the expected cumulative deposition density of global fallout from atmospheric nuclear weapons testing due to an enhanced scavenging effect. The 240Pu/239Pu atom ratios in the sediment core ranged from 0.239 to 0.246 with a mean value of 0.242 ± 0.002; these ratios were clearly greater than the mean global fallout ratio of 0.18. The results for 238Pu/239+240Pu activity ratios and 240Pu/239Pu atom ratios reflected a mixture of global fallout and Pacific Proving Grounds (PPG) close-in fallout Pu rather than Fukushima accident-derived Pu. The sediment column inventory for 239+240Pu originating from the PPG close-in fallout was calculated as 166 Bq m−2, which corresponded to 43% of the total inventory. A significant amount of the PPG-derived Pu has been transported by ocean currents and then preferentially scavenged in the coastal waters of Japan.

Migration path and isotope tracing of 137Cs and 239 + 240Pu in estuary sediments: a case study of Liao River estuary in China

Currently, the distribution characteristics and transport processes of the radionuclides 137Cs and 239 + 240Pu in the sediments of estuaries are still a controversial issue. Thus, in the present study, we investigated the distribution characteristics, sources and migration path of 137Cs and 239 + 240Pu in sediment cores of the Liao River estuary (LRE), China, and evaluated the relative contributions of the Pacific Proving Grounds (PPG) and riverine sources of Pu for the sediments in this area. We used 137Cs and Pu isotopes for dating the sediments and estimated the sedimentation rates by the two radionuclides in the LRE. Seven sediment samples were collected using a box corer from the Liao River estuarine wetland and tidal flat in the LRE in October 2012 and April 2015, respectively. The activities of 137Cs in the various samples were determined by γ spectrometry using HP-Ge detectors with 60% relative counting efficiency. Approximately 2–5 g of sediment were spiked with 242Pu (ca. 1 mBq) as a chemical yield tracer for Pu isotopic analysis at the School of Radiation Medicine and Protection, Soochow University. The measurement of Pu isotopes (239Pu, 240Pu, 242Pu) was performed by a sector field ICP-MS. In order to quantitatively differentiate the relative proportions of global fallout and PPG, we employed a two-end member mixing model to estimate their contributions. The average values of 137Cs, 239 + 240Pu activity concentrations, and 240Pu/239Pu atom ratios in the surface sediment samples of the LRE were 6.727 ± 0.251 mBq g−1, 0.294 ± 0.024 mBq g−1, and 0.188 ± 0.049 (1σ), respectively. The average 240Pu/239Pu atom ratios ranged from 0.180 ± 0.034 to 0.199 ± 0.021 in sediment cores from the east and west sides of the LRE. For core LT-2 values for 137Cs and 239 + 240Pu concentrations were from below the detection limit: 3.380 ± 0.414 and 0.036 ± 0.007 to 0.105 ± 0.007 mBq g−1. The mean 240Pu/239Pu atom ratio 0.217 ± 0.050 (1σ) in sediment core LT-2 lies between the global fallout and PPG close-in fallout. We found that atmospheric fallout is the main source of Pu in sediment cores from the east and west sides of the LRE. For core LT-2, atmospheric fallout and riverine input (~ 73.4%) are the major sources of Pu with the source of the rest of Pu (~ 26.6%) attributed to the PPG via the Tsushima Warm Current and the coastal water of the East China Sea. The sedimentation rates (means 0.62–0.8 cm year−1) estimated by the two radionuclides were in good agreement and without any statistically significant difference.

Spatial and temporal distribution of Pu in the Northwest Pacific Ocean using modern coral archives

Historical 239Pu activity concentrations and 240Pu/239Pu atom ratios were determined in skeletons of dated modern corals collected from three locations (Chuuk Lagoon, Ishigaki Island and Iki Island) to identify spatial and temporal variations in Pu inputs to the Northwest Pacific Ocean. The main Pu source in the Northwest Pacific is fallout from atmospheric nuclear weapons testing which consists of global fallout and close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands. PPG close-in fallout dominated the Pu input in the 1950s, as was observed with higher 240Pu/239Pu atom ratios (>0.30) at the Ishigaki site. Specific fallout Pu contamination from the Nagasaki atomic bomb and the Ivy Mike thermonuclear detonation at the PPG were identified at Ishigaki Island from the 240Pu/239Pu atom ratios of 0.07 and 0.46, respectively. During the 1960s and 1970s, global fallout was the major Pu source to the Northwest Pacific with over 60% contribution to the total Pu. After the cessation of the atmospheric nuclear tests, the PPG again dominated the Pu input due to the continuous transport of remobilised Pu from the Marshall Islands along the North Equatorial Current and the subsequent Kuroshio Current. The Pu contributions from the PPG in recent coral bands (1984 onwards) varied over time with average estimated PPG contributions between 54% and 72% depending on location.

Determination of 240Pu/239Pu atom ratio in seawaters from the east China sea

The (240)Pu/(239)Pu atom ratios in seawater samples on the East China Sea continental shelf were measured. These ratios for surface and bottom waters had no significant difference. They were significantly higher than the average global fallout ratio of 0.18. It was proposed that the oceanic currents are accounted for delivery of close-in Pu from the Pacific Proving Grounds (PPG) to the studied areas. The contribution of the PPG close-in fallout was calculated to be 40 % on average. The (240)Pu/(239)Pu atom ratios should provide useful background data before the expected expansion of nuclear power capacity in East and South Asian countries and for distinguishing future sources of Pu.

Pu and137Cs in the Yangtze River Estuary Sediments: Distribution and Source Identification

Pu isotopes and (137)Cs were analyzed using sector field ICP-MS and γ spectrometry, respectively, in surface sediment and core sediment samples from the Yangtze River estuary. (239+240)Pu activity and (240)Pu/(239)Pu atom ratios (>0.18) shows a generally increasing trend from land to sea and from north to south in the estuary. This spatial distribution pattern indicates that the Pacific Proving Grounds (PPG) source Pu transported by ocean currents was intensively scavenged into the suspended sediment under favorable conditions, and mixed with riverine sediment as the water circulated in the estuary. This process is the main control for the distribution of Pu in the estuary. Moreover, Pu is also an important indicator for monitoring the changes of environmental radioactivity in the estuary as the river basin is currently the site of extensive human activities and the sea level is rising because of global climate changes. For core sediment samples the maximum peak of (239+240)Pu activity was observed at a depth of 172 cm. The sedimentation rate was estimated on the basis of the Pu maximum deposition peak in 1963-1964 to be 4.1 cm/a. The contributions of the PPG close-in fallout Pu (44%) and the riverine Pu (45%) in Yangtze River estuary sediments are equally important for the total Pu deposition in the estuary, which challenges the current hypothesis that the riverine Pu input was the major source of Pu budget in this area.

Sources of plutonium to the tropical Northwest Pacific Ocean (1943–1999) identified using a natural coral archive

The Pu isotopes, 239Pu and 240Pu, were determined in annually-banded skeletons of an accurately dated (1943–1999) modern coral ( Porites lobata) from Guam Island to identify historical Pu sources to the tropical Northwest Pacific Ocean. Activity concentrations of 239+240Pu and 240Pu/ 239Pu atom ratios were determined in the dated coral bands using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands and global fallout were identified as the two main sources. The Guam site was dominated by PPG close-in fallout in the 1950s, with an average 240Pu/ 239Pu atom ratio of 0.315 ± 0.005. In addition, a higher 240Pu/ 239Pu atom ratio (0.456 ± 0.020) was observed that could be attributed to fallout from the “Ivy Mike” thermonuclear detonation in 1952. The atom ratio decreased in the 1960s and 1970s due to increase in the global fallout with a low 240Pu/ 239Pu atom ratio (∼0.18). Recent coral bands (1981–1999) are dominated by the transport of remobilised Pu, with high 240Pu/ 239Pu atom ratios, from the Marshall Islands to Guam Island along the North Equatorial Current (NEC). This remobilised Pu was estimated to comprise 69% of the total Pu in the recent coral bands, although its contribution was variable over time.

Concentrations of 137Cs, 90Sr, 108mAg, 239+240Pu and atom ratio of 240Pu/239Pu in tanner crabs, Chionoecetes japonicus and Chionoecetes opilio collected around Japan

The anthropogenic radionuclides, 137Cs, 90Sr, 108mAg, 239+240Pu, were measured in two Chionoecetes species, red queen crab (Chionoecetes japonicus) and snow crab (Chionoecetes opilio) collected around Japan during 1996–2007. There was no increase in the concentrations of these radionuclides and no large variation of the atom ratio of 240Pu/239Pu during this research period. These results indicated that the source of the radionuclides was not the radioactive wastes dumped by the former USSR and Russia and originated from past nuclear weapon tests. The higher atom ratio in the crab species than that from global fallout would be contributed by the Pacific Proving Grounds close-in fallout. The variability of the concentration of radionuclides in the crab species would result from the variability of the composition and quantity in the diet. However, the decrease in the concentration of radionuclides with sampling depth would depend on the concentration in the seawater and diet.

137Cs, 239+240Pu concentrations and the 240Pu/ 239Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of 137Cs and plutonium (Pu) isotopes. The 137Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the 137Cs and 239+240Pu. The shape of the vertical 137Cs distribution in the sediment core was similar to that of the Pu. The maximum 137Cs and 239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average 240Pu/ 239Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the 240Pu/ 239Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The 137Cs and 239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m 2 and 407 ± 27 Bq/m 2, respectively. Approximately 40% of the 239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure 240Pu/ 239Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.

Determination of 240Pu/ 239Pu atom ratio in coastal surface seawaters from the western North Pacific Ocean and Japan Sea

Surface seawater samples were collected from a site in the vicinity of the nuclear fuel reprocessing facility at Rokkasho, Japan and sites along the Japan Sea coast. 239+240Pu activities and 240Pu/ 239Pu atom ratios were determined by α-spectrometry and isotope-dilution sector-field ICP-MS. The 240Pu/ 239Pu atom ratio with the mean value of 0.227±0.006 was significantly higher than the mean global fallout ratio of 0.18. The contribution of the Pacific Proving Grounds close-in fallout was estimated to be 33% of the 239+240Pu.

240Pu/ 239Pu atom ratios in seawater from Sagami Bay, western Northwest Pacific Ocean: sources and scavenging

Seawater samples were collected in Sagami Bay, western Northwest Pacific Ocean, and their 239+240Pu activities and 240Pu/ 239Pu atom ratios were determined by α-spectrometry and sector field high-resolution ICP-MS. A few samples also were analyzed for 137Cs activities. The 239+240Pu inventory of 41.1 Bq m −2 was equivalent to the expected cumulative deposition density of atmospheric global fallout at the same latitude and this inventory was considerably lower than inventories in the underlying sediment columns. This result indicated that a significant amount of 239+240Pu has been removed into the underlying sediments through enhanced scavenging from the water column by the high fluxes of particles in this region. The atom ratio of 240Pu/ 239Pu showed no notable variation from the surface to the bottom; the average value was 0.234 ± 0.004. This atom ratio was significantly higher than the mean global fallout ratio of 0.18, proving the existence of close-in fallout plutonium originating from the Pacific Proving Grounds (PPG). The relative contributions of the global stratospheric fallout and the PPG close-in fallout were evaluated by using the two end-member mixing model. The contribution of the PPG close-in fallout was estimated to be 15.2 Bq m −2, which corresponded to 37% of the 239+240Pu inventory in the water column. Thus 239Pu and 240Pu from the two sources of global fallout and close-in fallout have been homogenized in the water masses in the western Northwest Pacific margin during the past three decades.

137Cs, 239 + 240 Pu and 240Pu / 239Pu atom ratios in the surface waters of the western North Pacific Ocean, eastern Indian Ocean and their adjacent seas

Surface seawater samples were collected along the track of the R/V Hakuho-Maru cruise (KH-96-5) from Tokyo to the Southern Ocean. The 137Cs activities were determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas, the eastern Indian Ocean, the Bay of Bengal, the Andaman Sea, and the South China Sea. The 137Cs activities showed a wide variation with values ranging from 1.1 Bq m − 3 in the Antarctic Circumpolar Region of the Southern Ocean to 3 Bq m − 3 in the western North Pacific Ocean and the South China Sea. The latitudinal distributions of 137Cs activity were not reflective of that of the integrated deposition density of atmospheric global fallout. The removal rates of 137Cs from the surface waters were roughly estimated from the two data sets of Miyake et al. [Miyake Y, Saruhashi K, Sugimura Y, Kanazawa T, Hirose K. Contents of 137Cs, plutonium and americium isotopes in the Southern Ocean waters. Pap Meteorol Geophys 1988;39:95–113] and this study to be 0.016 yr − 1 in the Sulu and Indonesian Seas, 0.033 yr − 1 in the Bay of Bengal and Andaman Sea, and 0.029 yr − 1 in the South China Sea. These values were much lower than that in the coastal surface water of the western Northwest Pacific Ocean. This was likely due to less horizontal and vertical mixing of water masses and less scavenging. 239 + 240 Pu activities and 240Pu / 239Pu atom ratios were also determined for the surface waters in the western North Pacific Ocean, the Sulu and Indonesian Seas and the South China Sea. The 240Pu / 239Pu atom ratios ranged from 0.199 ± 0.026 to 0.248 ± 0.027 on average, and were significantly higher than the global stratospheric fallout ratio of 0.18. The contributions of the North Pacific Proving Grounds close-in fallout Pu were estimated to be 20% for the western North Pacific Ocean, 39% for the Sulu and Indonesian Seas and 42% for the South China Sea by using the two end-member mixing model. The higher 240Pu / 239Pu atom ratios could be attributed to close-in fallout Pu delivered from the Enewetak and Bikini Atolls by ocean currents of branches of the North Equatorial Current to the Southeast Asian seas.