239, 240Pu,137Cs and90Sr in the central North Pacific

^{239, 240}Pu,¹³⁷Cs and⁹⁰Sr concentrations were determined in sea waters from the central and western North Pacific in 1980 and 1982. The results are consistent with those reported earlier for North Pacific waters. The profiles of⁹⁰Sr and¹³⁷Cs show a monotonic decrease with depth, whilst^{239, 240}Pu shows a distinct subsurface maximum at a depth between 400 and 1,000 m. The calculated inventories of these nuclides significantly exceed the global mean fallout inputs for these latitudes. This may be due to local fallout input to the ocean at times of large-scale nuclear weapon tests in the equatorial North Pacific. The existence of measurable amounts of¹³⁷Cs and^{239, 240}Pu in deep waters suggests that these nuclides are transported by sinking particulate matter from the surface to the deep ocean.     

Artificial radionuclides in the western Northwest Pacific (I)90Sr and137Cs in the deep waters

⁹⁰Sr and¹³⁷Cs concentrations and their vertical distributions were determined in deep waters in the western Northwest Pacific, including the adjacent seas of Japan, from 1976 to 1979.The profiles of the radionuclides show distribution patterns with two parts with an exponential variation of radioisotope content with depth in both parts.Generally speaking, the inventories of⁹⁰Sr and¹³⁷Cs in the open waters of the northwestern Pacific correspond fairly well to the fallout inputs, but in some circumstances there seems to be considerable removal of radionuclides from the water column or they are diluted with water of lower radioactivity from other regions.The possibility of radioisotope remobilization from the bottom sediment or particulate matter is also discussed.     

Artificial radionuclides in the western Northwest Pacific (II):137Cs and239,240Pu inventories in water and sediment columns observed from 1980 to 1986

Concentrations and inventories of¹³⁷Cs and^239,240Pu were determined in sea waters and sediments columns from the western North Pacific from 1980 to 1986.The^239,240Pu/¹³⁷Cs activity ratio in the water column shows a tendency to increase from the surface (10^–3) to bottom waters (10^–1), but the ratio in sediment is within a rather narrow range (10^–2 to 10^–1), indicating more effective removal of plutonium from the water column than¹³⁷Cs. In regions south of 40N, the radionuclide inventories in the water column significantly exceed the estimated global fallout (stratospheric fallout due to the atmospheric nuclear explosion), especially in the case of^239,240Pu. These excess inventories imply that local or close-in fallout derived from nuclear explosions in the equatorial North Pacific are well-preserved and retained in the regions, despite about 20 years since the atmospheric nuclear explosion moratorium. Data suggesting lateral transport of¹³⁷Cs in surface water from north of 40N to southern regions is shown. Some data on⁹⁰Sr contents are also shown.     

Preliminary report on radionuclide concentrations in the bottom waters at the entrance of Wakasa Bay with special reference to the Japan Sea Proper Water

Marked fluctuation of concentrations of⁹⁰Sr and¹³⁷Cs was observed in the bottom waters at the entrance of Wakasa Bay during 1987–1992, and the cause was investigated. The concentrations of⁹⁰Sr and¹³⁷Cs in the bottom waters were significantly low when the upper level of the Japan Sea Proper Water (JSPW) was high and covered the sampling depth, but high when the upper level of the JSPW was low. The cause of the fluctuation observed in the bottom waters is, therefore, suggested to be the vertical fluctuation of the upper level of the JSPW on the shelf slope, which has been little described before.     

Forty years of anthropogenic radionuclides in surface seawater. Italian and Japanese data

The concentrations of man made radionuclides in surface seawater since early ′60s are here reported as measured in Italy and Japan. Most of the data refers to⁹⁰Sr and¹³⁷Cs, but occasionally the concentrations of⁸⁹Sr and¹³⁴Cs in some Italian samples are also given. The main sources of man made radionuclides were the global fallout produced by the nuclear weapon tests and the Chernobyl accident. The respective contributions to the contamination of surface seawater around both countries are discussed.     

Numerical experiment for strontium-90 and cesium-137 in the Japan Sea

A numerical experiment is carried out to reproduce distribution of concentration of ⁹⁰Sr and ¹³⁷Cs, estimate their total amount and verify their source in the Japan Sea. Model results are in good agreement with observational findings in the Japan Sea expeditions between 1997 and 2002 by the Japan Atomic Energy Agency. Vertical profiles of the concentration of ⁹⁰Sr and ¹³⁷Cs show exponential decreases with depth from the sea surface to the sea bottom. From the model and observational results, it is suggested that the concentration of ⁹⁰Sr and ¹³⁷Cs in the surface layer is approximately in the range of 1.0–1.5 Bq/m³ and 2.0–2.5 Bq/m3, respectively. On the other hand, it is found that the concentration in the intermediate and deep layer is higher than that observed in the northwestern Pacific Ocean, suggesting active winter convection in the Japan Sea. The total amount of ⁹⁰Sr and ¹³⁷Cs in the seawater is evaluated to be 1.34 × 10¹⁵ Bq and 2.02 × 10¹⁵ Bq, respectively, in the numerical experiment, which demonstrates an estimation by observational data obtained in the Japan Sea expeditions. The total amount of ⁹⁰Sr and ¹³⁷Cs changed during the second half of 20th century corresponding to deposition at the sea surface with the maximums of 4.86 × 10¹⁵ Bq for ⁹⁰Sr and 7.33 × 10¹⁵ Bq for ¹³⁷Cs, respectively, in the mid-1960s. The numerical experiment suggests that the main source of ⁹⁰Sr and ¹³⁷Cs has been global fallout, although there have been some potential sources in the Japan Sea.     

Dispersion and accumulation of radionuclides in sediment of Urazoko Bay (I)

Contents of⁹⁰Sr,¹³⁷Cs and⁶⁰Co in surface sediments were investigated in and around Urazoko Bay, Fukui Prefecture, where a nuclear power plant has been operating since 1969 and the waste effluent has been released into the sea. The main source of⁹⁰Sr and¹³⁷Cs was recognized to be radioactive fallout, whereas⁶⁰Co was considered to originate from the nuclear power plant. Using the¹³⁷Cs concentration as an indicator of sorption capacity of the sediment, the behaviour of⁶⁰Co was investigated. No seasonal variation was observed in the distribution pattern of⁶⁰Co/¹³⁷Cs ratio and the retention of the heavy initial discharge in 1969 was considered to dominate the radionuclide level in the sediment. Correlation of⁶⁰Co/¹³⁷Cs ratio in the sediment and the distance from the discharge outlet was expressed by a simple exponential function of the distance. It was suggested that the contamination is spreading out gradually to the outer region of Urazoko Bay.     

Activity Concentrations and Fluxes of Radiocesium in the Southern Baltic Sea

The activity concentrations of dissolved¹³⁷Cs have been determined in the water column and¹³⁷Cs and¹³⁴Cs in the sediments and the sediment porewaters of the southern Baltic Sea. The mean activity concentration of dissolved¹³⁷Cs in the Gdansk Deep declined from 109 Bq m⁻³in June 1986 to 61 Bq m⁻³in 1999. In sediments, the activity concentrations of¹³⁷Cs (33-231 Bq kg⁻¹) were highest in muds and the activity concentrations of¹³⁴Cs were about 6% of the total Cs activity. The Chernobyl contribution to¹³⁷Cs activity was between 43% and 77%. The porewater activity concentrations of¹³⁷Cs in muddy sediments were in the range 71 to 3900 Bq m⁻³and were higher than those in the overlying seawater. The diffusive flux of dissolved¹³⁷Cs from the muddy sediments was estimated in the range 5 to 480 Bq m⁻²year⁻¹. The flux of¹³⁷Cs from sediment porewaters of the southern Baltic Sea was about 45% of the total, including fluxes of¹³⁷Cs from wet and dry atmospheric deposition and the fluvial inputs. The results were used to elucidate the rate of recovery of the sediments and the waters of the southern Baltic from Chernobyl-derived¹³⁷Cs.     

Radioactive isotopes of caesium in the waters and near-water atmospheric layer of the Black Sea

The concentrations of¹³⁷Cs and¹³⁴Cs were measured using the sorption method in the waters of the Black Sea during 1986–1987. An inhomogeneous character of the contamination of the surface waters in the Black Sea due to the Chernobyl disaster is shown. The subsequent migration and redistribution of caesium radionuclides in the various seasons of the year were studied. The amount of¹³⁷Cs and¹³⁴Cs in the upper 50 m layer was estimated. The results of measuring the concentration of caesium radionuclides in the near-water atmospheric layer over the Black Sea and Mediterranean Sea in 1986–1987 are also reported.Translated by Mikhail M. Trufanov.     

The process of self-purification of the Baltic Sea waters from artificial radionuclides

An analysis of the variations in the concentrations of ¹³⁷Cs and ⁹⁰Sr radionuclides in the Baltic Sea surface waters after the accident at the Chernobyl nuclear power plant was performed. An instability of the ¹³⁷Cs concentration values during the short-term observations was found, when these values were differed 2-to 3-fold. The concentrations of ⁹⁰Sr appeared to be more stable; meanwhile, their deviations sometimes exceeded the ranges of the experimental errors. By the variations in the monthly average values of the radionuclide concentrations in the surface waters of the Baltic Sea in 1989–1995, no trend of the water self-purification was observed. The theoretical results obtained confirmed the potential of the formation and propagation of patches with increased concentrations of ¹³⁷Cs in the southeastern part of the Baltic Sea. The most reliable factor that controlled the process of self-purification of the Baltic Sea water appeared to be the mean annual value of the concentration of radionuclides. Pronounced divergences were obtained between the measured and calculated mean annual concentrations of ¹³⁷Cs and ⁹⁰Sr radionuclides in the surface waters of the Baltic Sea in 1989–2001. These divergences are explained by the potential influence of the waters from the Gulf of Bothnia and by other additional supplies of radionuclides to the marine environment, which were not included into the mathematical models.     

福岛核事故泄漏入海的137Cs长期输运的数值研究

The Fukushima nuclear accident in 2011 released large amounts of radionuclides, including ~(137)Cs, into the Pacific Ocean. A quasi-global ocean radioactive transport model with horizontal grid spacing of 0.5°×0.5° and 21 vertical layers was thereafter established to study the long-term transport of the Fukushima-derived ~(137)Cs in the ocean.The simulation shows that the plume of ~(137)Cs would be rapidly transported eastward alongside the Kuroshio Current and its extensions. Contaminated waters with concentrations lower than 2 Bq/m3 would reach the west coast of North America 4 or 5 years after the accident. The ~(137)Cs tends to be carried, despite its very low concentration, into the Indian and South Pacific Oceans by 2016 via various branches of ocean currents.Meanwhile, the ~(137)Cs concentrations in the western part of the North Pacific Ocean decrease rapidly with time. Up to now the highly contaminated waters have remained in the upper 400 m, showing no evidence of significant penetration to deeper layers.     

A field study of physico-chemical states of artificial radionuclides in seawater

The physico-chemical states of artificial radionuclides,⁹⁰Sr,¹³⁷Cs and¹⁴⁴Ce in seawater were investigated by radiochemical analysis of filtered and unfiltered seawater. The difference of radionuclide concentrations between unfiltered and filtered seawaters was defined as the particulate form radioisotope and its particle ratio was discussed.Practically no particulate⁹⁰Sr, greater than 0.22 in size, was observed in both coastal and open seawaters, but some of¹³⁷Cs seemed to be insoluble in some circumstances, especially in coastal waters. A considerable amount of¹⁴⁴Ce was found to be particulate.An estimation of the radionuclides in particulate form was made for Kashima-nada seawaters collected in 1970 to 1972, and it was shown that the possible occurrence of particulate radionuclides, greater than 0.22 in size, were 1% or less for⁹⁰Sr and 6% for¹³⁷Cs. In the coastal water, 80 % of¹⁴⁴Ce were seemed to be in particulate form, but in the open seawater only a few%. The influences of suspended materials to¹³⁷Cs and¹⁴⁴Ce concentration levels in seawater were not negligible and further investigations are desirable.     

The transfer of reprocessing wastes from north-west Europe to the Arctic

The discharge of radioactive waste, from nuclear fuel reprocessing facilities, into the coastal waters of north-west Europe has resulted in a significant increase in the inventories of a number of artificial radionuclides in the North Atlantic. Radiocaesium, ⁹⁰Sr and ⁹⁹Tc, which behave conservatively in seawater, have been used widely as tracers of water movement through the North Sea, Norwegian Coastal Current, Barents Sea, Greenland Sea, Fram Strait, Eurasian Basin, East Greenland Current and Denmark Strait overflow. These studies are summarised in the present paper. It has been estimated that 22% of the ¹³⁷Cs Sellafield discharge has passed into the Barents Sea, en route to the Nansen Basin, via the Bjomoya-Fugloya Section, with another 13% passing through the Fram Strait. This amounts to 14 PBq ¹³⁷Cs. Quantifying the influx of other radionuclides has been more problematic. The inflowing Atlantic water now appears to be diluting waters in the Arctic Basin, which were contaminated in the late 1970s and early 1980s as a result of the substantial decrease in the discharge of reprocessing wastes. Sellafield (U.K.) has dominated the supply of ¹³⁴Cs, ¹³⁷Cs, ⁹⁰Sr, ⁹⁹Tc and Pu, whereas La Hague (France) has contributed a larger proportion of ¹²⁹I and ¹²⁵Sb.     

Methane in the western North Pacific

The concentration of methane in about 400 seawater samples collected in the western North Pacific, mostly from 40°N to 5°S along 165°E was determined. While the concentration of methane in the surface water was slightly greater in the high-latitudes, it did not widely vary with a standard deviation of 0.29 n mol/l for a mean value of 2.49 n mol/l. The 90% confidence limit of the mean was 0.08 n mol/l. The degree of oversaturation in 1991 (31±4%) was not different from that in circa 1970. If we assume that this degree of oversaturation occurs in the entire oceans, the annual flux of methane becomes 6×10¹²g CH₄. Both the concentrations of methane and chlorophylla were higher in the surface 100 m layer. However, the correlation between them was not well in the entire surface waters. This may indicate that the production of methane is not directly related to the photosynthetic process. The concentration of methane decreased gradually with increasing depth down to 1000 m. Its horizontally and vertically uniform concentration in the abyssal water suggests that the turnover time of methane in the oxic pelagic water is in the range between a few years and a few hundred years.     

Fluxes of234Th,210Po and210Pb determined by sediment trap experiments in pelagic oceans

Sediment trap experiments were carried out in two oceans, the eastern Pacific Ocean and the Antarctic Ocean, which have very different biological productivities. The natural radionuclides,²³⁴Th,²¹⁰Po and²¹⁰Pb were used as tracers of reactive metals. Larger particulate fluxes of these radionuclides were found in the seas where total mass fluxes were larger, although the concentrations of these radionuclides in the settling particles were somewhat smaller. The concentrations of²³⁴Th in the settling particles varied widely and irregularly with depth, whereas the concentrations of²¹⁰Po and²¹⁰Pb in the settling particles steadily increased with increasing water depth. The ratios of²¹⁰Po/²¹⁰Pb in the settling particulates were larger than unity which the ratio of²³⁴Th/excess²¹⁰Po as larger than²³⁴Th/²¹⁰Po in the deep water. These results suggest that, when the particles sink through the water column, these radionuclides are being absorbed by settling particles in the order²³⁴Th>²¹⁰Po>²¹⁰Pb. The observed particulate fluxes of²¹⁰Pb are about one eighth of those calculated from the disequilibria between²²⁶Ra and²¹⁰Pb at the stations in the subtropical eastern Pacific, although the observed fluxes are the same as the calculated ones in the northern North Pacific and the Antarctic Ocean. Thus, there must be a horizontal flow carrying these reactive metals from the oligotorophic ocean to the biologically productive ocean where the metals are removed by settling particles even in deep water.     

Distribution and inventories of 90Sr, 137Cs, 241Am and Pu isotopes in sediments of the Northwest Pacific Ocean

Bottom sediments collected in the Northwest (NW) Pacific Ocean in 1997 were analysed for ⁹⁰Sr, ¹³⁷Cs, ^239,240Pu and ²⁴¹Am contents to determine their distribution patterns, inventories and sources. Enhanced inventories of ^239,240Pu and ²⁴¹Am were observed in the latitudinal belts of 10–20°N and 30–40°N, which correspond to major areas of local (tropospheric) and global (stratospheric) fallout (with a contribution from local fallout), respectively. The sediment inventory of ^239,240Pu near the Bikini Atoll exceeded its overlying water inventory, however, in the mid-latitudes, more than 70% of ^239,240Pu still remains in the water column. ²⁴¹Am inventories in sediments exceeded that of the water column for the entire NW Pacific Ocean. Higher ¹³⁷Cs and ⁹⁰Sr sediment inventories in the latitudinal belt of 30–40°N are due to global fallout, and they account for about 10% and less than 5% of the water column inventories, respectively. The observed activity ratios of ¹³⁷Cs/⁹⁰Sr, ²³⁸Pu/^239,240Pu and ²⁴¹Am/^239,240Pu in sediment were at some stations higher than the global fallout ratios due to contributions from local fallout and due to specific processes in the water column. Two end-member mixing model based on the ²⁴⁰Pu/²³⁹Pu atom ratios observed in global and local fallout yielded ∼60% contribution of the local fallout in the bottom sediments near the Bikini Atoll. The upward decrease in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment column indicates a decrease in the contribution of local fallout to the Pu inventory with time. ²⁴¹Am and ²⁴¹Pu dating of sediment layers was utilized to explain a hiatus in sediment accumulation in the deep seafloor.     

Contents of strontinm-90 and ruthenium-106 in beach and shallow water deposits of noto peninsula

⁹⁰Sr,¹⁰⁶Ru, natural strontium and major elements were studied in 12 samples of beach deposits from Togi, Fukuura and Shiga, and in 26 samples of shallow water sediments from sea off Fukuura, Noto Peninsula, Ishikawa Pref., Japan.The average contents of natural strontium and⁹⁰Sr in the beach deposits were 488 ppm ranging from 247 to 1,550 ppm and 45±9 pCi kg^–1-dry mud ranging from 18 to 72 pCi kg^–1-dry mud, respectively. While the average contents of natural strontium,⁹⁰Sr and¹⁰⁶Ru in the sediments were 234 ppm ranging from 136 to 415 ppm, 22±6 pCi kg^–1-dry sand ranging from 7 to 48 pCi kg^–1-dry sand and 0.6 ±0.2 nCi kg^–1-dry ranging from 0.3 to 1.2 nCi kg^–1-dry, respectively.The average contents of each natural strontium and⁹⁰Sr in the beach deposits were about two times higher than those in the shallow water sediments. But no obvious relation of natural strontium to⁹⁰Sr was found in all the samples. The enrichment of⁹⁰Sr and¹⁰⁸Ru in the beach deposits or tthe sediments were as high as 150320 and of 2,0003,000 compared with average contents of⁹⁰Sr and¹⁰⁶Ru in a liter of surface water from the Japan Sea. It is to be noticed that the average¹⁰⁶Ru to⁹⁰Sr ratio of 27 for the shallow water sediments is much higher than the average of 1.0 for surface sea water of the Japan Sea.As to major elements of the samples, the beach deposits are rich in silicon (Av. 70.89 ±0.92% SiO₂), but poor in iron (Av. 2.99±0.32% Fe₂O₃). Whereas the shallow water sediments are poor in silicon (Av. 52.96±10.33% SiO₂) and rich in iron (Av. 5.50±1.90% Fe₂O₃), calcium (Av. 9.64±9.22% CaO) and magnesium (Av. 2.83±1.58% MgO).     

224,223Ra和137Cs在吕宋海峡及周边海域的分布以及其对“彩虹”台风的响应

本文报道2015年9月和2016年5月期间天然放射性核素²²⁴Ra和²²³Ra在吕宋海峡及周边海域表层和垂向水体的分布特征。为理解日本福岛核事故的影响,本文亦分析研究区域内人工放射性核素¹³⁷Cs的分布特征。结果表明,^224,223Ra和¹³⁷Cs比活度水平均处于我国南海海洋天然放射性本底变化范围之内。²²⁴Ra在吕宋海峡以西南海北部海域比活度较高,在吕宋海峡以东菲律宾海域比活度较低。¹³⁷Cs没有明显的分布趋势。基于三站位（LS3,LS5和LS8）²²⁴Ra、¹³⁷Cs以及温盐的垂向分布特征,本文揭示²²⁴Ra和¹³⁷Cs在热带表层水、次表层水和中-深层水中比活度水平和梯度变化的差异特征。彩虹台风事件扭转了整个吕宋海峡及周边海域的海流循环过程。大量以低水平²²⁴Ra为特征的西太平洋海水涌入南海,降低水体²²⁴Ra比活度水平。但是,西太平洋和南海北部海域水体¹³⁷Cs比活度水平没有明显差异,台风导致的海流变化对水体¹³⁷Cs比活度没有明显影响。     

239,240Pu and137Cs in the East China and the Yellow Seas

The distribution and inventory of artificial radionuclides,^239,240Pu and¹³⁷Cs were determined in the East China and the Yellow Seas in 1987. Almost all of^239,240Pu and 50 to 80% of¹³⁷Cs in the continental shelf area are retained in the sediment column.^239,240Pu sediment inventory in the sea area is larger than the fallout input and tends to increase southwardly. This excess^239,240Pu and the lateral distribution are attributable to the supply of^239,240Pu by the Yangtze River discharge. On the contrary,¹³⁷Cs sediment inventory shows a decrease to the south, and the fact can be accounted for by the southward dispersion of fine silt particles discharged from the Yellow River. Total¹³⁷Cs inventory is smaller than the estimated fallout input, and the fact seems to indicate dispersion of¹³⁷Cs out of the shelf region. Vertical profiles of^239,240Pu and¹³⁷Cs contents in sediments differ from that of natural²¹⁰Pb, implying the effect of varied accumulation rates of the artificial radionuclides over the sediment particle mixing by benthic organisms. Apparent maximum sediment particle mixing coefficient (D _B ) calculated from the excess²¹⁰Pb profiles in stations located between the inner and outer shelves ranged from 1.4 to 8.3 cm²y^–1. ThisD _B value is higher than that in the Okinawa Trough (1.0 cm²y^–1), but lower than previously estimatedD _B value (26 cm²y^–1) in the outer shelf mud.     

海洋中90Sr:日本周边海域与南海的对比

90Sr长期被视为最重要的人工放射性核素之一,日本福岛核事故导致包括90Sr在内的大量放射性物质泄漏进入海洋,厂区储水罐中冷却废水至今仍然存在大量90Sr。海洋中90Sr分析方法却繁琐耗时,导致核事故后的90Sr研究较为匮乏,且缺乏系统的认识。本研究在2015?2018年期间测量南海海水和多种海洋生物(马尾藻、海虾、牡蛎、红树林植物、造礁珊瑚)中90Sr的基础上,深入分析核事故后日本周边海域和南海90Sr的比活度水平与环境半衰期。结合文献资料,本研究发现1975?2010年期间日本近岸海水90Sr的环境半衰期为15.4 a,2011年的核事故后日本周边海洋中90Sr比活度显著升高,基于ERICA软件定量计算核事故后90Sr对海洋鱼类的剂量率比核事故前的结果高5个数量级。南海作为福岛核事故后北太平洋环流的下游海域,本文进一步构建1984?2018年期间南海90Sr比活度的历史曲线,发现核事故前后南海90Sr比活度水平没有可识别的变化,进一步定量计算南海90Sr的环境半衰期为26.7 a,发现边缘海和大洋中90Sr和137Cs环境半衰期格局差异与核素(90Sr和137Cs)的源汇过程(河流输入和海洋生物泵)密切相关。鉴于海洋中90Sr分析方法的挑战性,本文发现在10多种海洋生物中造礁珊瑚骨骼几乎拥有最高的90Sr浓集因子(约1 000 L/kg),同时具有较易大量获取、固定附着生长、连续高分辨率记录、前处理简单快速等优点,很可能是海洋中90Sr可靠的指示生物。造礁珊瑚中90Sr研究将有利于揭示人工放射性核素的源汇过程,同时为我国海洋放射性监测方案和相关标准导则的优化和完善提供有益的参考。