Abstract
Deep-ocean sediments, similarly to seawater, are important reservoirs of
137
Cs, an anthropogenic radionuclide with a relatively long half-live found in the Earth system. To better ...understand the geochemical behaviour of
137
Cs in the ocean, we examined the temporal changes of
137
Cs activity concentrations in the overlying waters and in sediments from the Far Eastern Seas (Sea of Japan, SOJ, and Okhotsk Sea, OS) during the period of 1998–2021. The
137
Cs activity levels showed exponential changes during the observed period. The decay-corrected change rates of
137
Cs in deep waters of SOJ exhibited a slow increase, while
137
Cs levels in seawater and sediment in OS decreased gradually. This reflects a topographical difference, as SOJ is a semi-closed sea, whereas OS receives continuously inflow of subarctic waters. It was confirmed that
137
Cs released after the Fukushima Dai-ichi Nuclear Power Plant accident was rapidly transported into the deep waters of the SOJ. To elucidate the transfer processes of
137
Cs from seawater to sediment, we discussed the temporal changes of the partition coefficients (K
d
) of
137
Cs between the overlying water and the surface sediment. In shallow areas (< 1500 m water depth), K
d
values were almost constant within the sampling periods, although the temporal changes in the K
d
values occurred in deeper waters (> 2500 m depth). The K
d
values increased with increasing depth, which may reflect a pressure effect as a possible mechanism. These findings suggest that chemical processes may be important factors controlling the transport of
137
Cs between seawater and sediment, although more complicated phenomena occurred in deep waters and sediments of the SOJ (> 3000 m depth).
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
The impact of the Fukushima-derived radiostrontium (90Sr and 89Sr) on the western North Pacific Ocean has not been well established, although 90Sr concentrations recorded in surface seawater offshore ...of the damaged Fukushima Dai-ichi nuclear power plant were in some areas comparable to or even higher than (as those in December 2011 with 400 kBq m–3 90Sr) the 137Cs levels. The total amount of 90Sr released to the marine environment in the form of highly radioactive wastewater could reach about 1 PBq. Long-term series (1960–2010) of 90Sr concentration measurements in subtropical surface waters of the western North Pacific indicated that its concentration has been decreasing gradually with a half-life of 14 y. The pre-Fukushima 90Sr levels in surface waters, including coastal waters near Fukushima, were estimated to be 1 Bq m–3. To better assess the impact of about 4–5 orders of magnitude increased radiostrontium levels on the marine environment, more detail measurements in seawater and biota of the western North Pacific are required.
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In March 2011, severe nuclear accident happened at the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) after the gigantic earthquake and following huge tsunami wave. A lot of investigations to assess ...environmental and radiological impacts of released radionuclides have been conducted by domestic and international organizations. Environmental radioactivity research related to the FDNPP accident has spread widely over different scientific fields due to specific features of the accident, and specifically its impact on the marine environment. The present paper summarizes major lessons learned from the environmental investigations of the FDNPP accident. Environmental radioactivity studies have typical interdisciplinary character; especially physics and chemistry are fundamental as a base of process studies in the environment. In this sight, we review chemical aspects regarding FDNPP-derived radiocesium transfer within and between compartments (atmosphere, ocean and land). We also discuss future trends in investigations of behavior of anthropogenic radionuclides in the environment, important not only for a better understanding of impacts of the FDNPP accident on the environment, but also for improving our general knowledge of the total environment in the Anthropocene era and its protection for the future.
•10 years after the FDNPP accident, the environment has been contaminated mainly by Cs-137.•Understanding of Cs-transfer within and between compartments has considerably improved.•Chemical processes are a key factor of Cs-transfer between aquatic and solid phases.•Migration of Cs-137 in terrestrial and marine ecosystems will dominate in future studies.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The investigation of the impact of the Fukushima accident is still going on although more than ten years have passed since the disaster. The main goal of this paper was to summarize the results of ...tritium and radiocarbon determinations in different environmental samples, possibly connected with the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. A document containing compiled data may serve as a solid basis for further research in the selected fields. To accomplish such effort, we went through dozens of relevant published papers, reporting 3H and 14C activity concentrations in precipitations, groundwater, seawater, river systems, tree rings, and, in some more extraordinary samples, such as herbaceous plants or debris from the damaged reactor buildings. As the referenced results would not be obtainable without adequate analytical techniques, the most common methods for routine measurement of tritium and radiocarbon concentrations are discussed as well. We believe that the correct identification of the affected environmental compartments could help quantify the released 3H and 14C activities and track their following fate, which could be especially important for plans to discharge contaminated water from the FDNPP in the upcoming years.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Plutonium isotopes have primarily been injected to the stratosphere by the atmospheric nuclear weapon tests and the burn-up of the SNAP-9A satellite. Here we show by using published data that the ...stratospheric plutonium exponentially decreased with apparent residence time of 1.5 ± 0.5 years, and that the temporal variations of plutonium in surface air followed the stratospheric trends until the early 1980s. In the 2000s, plutonium and its isotope ratios in the atmosphere varied dynamically, and sporadic high concentrations of (239,240)Pu reported for the lower stratospheric and upper tropospheric aerosols may be due to environmental events such as the global dust outbreaks and biomass burning.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Recent developments in radiometric and mass spectrometry technologies have been associated in the radiometric sector mainly with underground operations of large volume Ge detectors, while the ...mass-spectrometry sector, represented mainly by accelerator mass spectrometry and inductively coupled plasma mass spectrometry has become the most sensitive technique for ultra-low-level analyses of long-lived radionuclides. These new developments have had great impact on investigations of rare nuclear processes and applications of radionuclides in environmental, life and space sciences. New scientific investigations have been carried out therefore which have not been possible before either because of lack of sensitivity or required large sample size.
Variations of Fukushima-derived radionuclides ((90)Sr, (134)Cs and (137)Cs) in seawater and biota offshore Fukushima and in the NW Pacific Ocean were investigated and radiation doses to the Japanese ...and world population from ingestion of seafood contaminated by Fukushima radionuclides were estimated and compared with those from other sources of anthropogenic and natural radionuclides. The total effective dose commitment from ingestion of radionuclides in fish, shellfish and seaweed caught in coastal waters off Fukushima was estimated to be 0.6 ± 0.4 mSv/y. The individual effective dose commitment from consumption of radioactive-contaminated fish caught in the open Pacific Ocean was estimated to be 0.07 ± 0.05 mSv/y. These doses are comparable or much lower than doses delivered from the consumption of natural (210)Po in fish and in shellfish (0.7 mSv/y). The estimated individual doses have been below the levels when any health damage of the Japanese and world population could be expected.
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The most sensitive technologies for ultra-low-level analyses of long-lived radionuclides have been accelerator mass spectrometry and inductively coupled plasma mass spectrometry, reaching detection ...limits about 1 nBq/g. Together with underground operation of large volume HPGe detectors they have had great impact on underground physics experiments, approaching new frontiers in radioanalytics—a single atom counting.
Long-term temporal variations of plutonium in Sea of Japan (SOJ) surface waters have been examined with the aim to better understand its behavior during several decades. The first observation is that ...239,240Pu activity concentrations in surface waters of the SOJ during 1977–2019 were 6.5 ± 4.7 mBq m−3 in average, and 5.1 mBq m−3 as the median, whereas 137Cs and 90Sr activity concentrations decreased with time, except of the perturbation due to the 2011 Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. Another observation is that sporadic high 239,240Pu activity concentrations occurred in the east Japan Basin, ranging from 1 to 39 mBq m−3. The spatial distribution of 239,240Pu activity concentrations in surface waters revealed that high 239,240Pu levels (>20 mBq m−3) occurred in 1994 in the northern SOJ, which was considered to be due to winter convection. To elucidate factors controlling the temporal variability of surface 239,240Pu levels in the SOJ, a relationship between surface 239,240Pu activity concentrations and vertical diffusion coefficients was examined. The results revealed that this relationship could be classified into two groups: one group did not show a change with increasing diffusion coefficient, while the other group showed a positive correlation. The vertical 239,240Pu distribution in SOJ waters suggests that the high surface 239,240Pu levels occurred due to the upwelling of cyclonic eddy. The rapid recycling of deeper plutonium occurred in the SOJ due to deep winter convection and upwelling associated with cyclonic eddy. The plutonium levels in the SOJ have been found to be sensitive to climate changes. Warming of the SOJ may cause a reduction of winter convection and eddy activity as a result of increasing sea surface temperature. This leads to a decline of recirculation of plutonium and other bioavailable elements from Japan Sea Proper Water (JSPW) to surface water layers. Plutonium would be, therefore, an important indicator of biogeochemical processes in the marine environment, helping to assess climate change impacts on marine ecological systems.
•Long-term variability of 239,240Pu activity concentrations in surface water in the Sea of Japan (SOJ) was examined.•The temporal change of surface 239,240Pu did not exhibit long-term exponential decrease.•In the SOJ, recirculation of 239,240Pu occurred from subsurface to surface in 1994 winter.•The winter convection and upwelling due to cyclonic eddy is related to recirculation of 239,240Pu in the SOJ.•Global warming affects oceanographic conditions in the SOJ and may be weakened recirculation of 239,240Pu.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
90Sr and 137Cs activity concentrations in surface waters of the Sea of Japan (SOJ) decreased during the period of 1993–2010 with effective half-lives of 18 and 15 y, respectively. The longer ...effective half-life of 90Sr in the SOJ may suggest a surplus of 90Sr to SOJ surface waters, however, no clear evidence of possible 90Sr source has been found. After the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, temporal variations of 137Cs in the surface water of the SOJ have changed, while 90Sr variations followed the pre-accident trends. The 90Sr/137Cs ratios reveal that increases of 137Cs due to the FDNPP accident continued in surface waters of the SOJ until 2016.
•137Cs and 90Sr are useful tracers for studying processes in the Sea of Japan (SOJ).•Effective half-life of 90Sr in surface water of the SOJ is longer than expected.•90Sr/137Cs activity ratios help to elucidate oceanic effects of the Fukushima accident.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
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