Radioecological behaviour of 137Cs in rockfish of the southern coastal waters off Fukushima during 2017-2021.

Following the accident at the Fukushima Dai-ichi Nuclear Power Station, radiocaesium concentrations were specifically elevated in rockfish species compared to other fish species. To clarify the likely reasons, a caesium metabolic rate in the Japanese rockfish Sebastes cheni was derived by an aquarium experiment of live fish collected from the area off Fukushima. Stable caesium and 137Cs concentration in prey organisms, stomach contents and muscle of rockfish were measured and the bioavailable fraction in prey organisms was evaluated. Using derived transfer parameters, 137Cs radioactivity levels in S. cheni and prey organisms were simulated by a model, and verified by the measured radioactivity concentrations of biota in coastal waters south of the Fukushima Dai-ichi Nuclear Power Station. As a result, slow caesium metabolism in S. cheni was confirmed with the biological half-life (Tb1/2) of 190 d. The determining factor for the initial 137Cs radioactivity levels in S. cheni, was the maximum radioactivity levels in surrounding seawater which was constrained by the sedentary nature of rockfish. Controlling factors of depuration rate of 137Cs levels in S. cheni were slow caesium metabolism, enhanced 137Cs radioactivity level of prey organisms, and survival of older contaminated individuals due to a long life-span. During the study period 2017-2021, 137Cs radioactivity concentrations in seawater decreased close to the level measured before 2010, whereas those in prey organisms and rockfish in southern Fukushima waters were still above the levels that existed before 2010. An additional source for enhancing 137Cs radioactivity in rockfish and biota of the food chain was indicated by the greater 137Cs/133Cs atom ratios in rockfish compared to those in the surrounding seawater, however it was considered to be radiologically insignificant in relation to seafood safety limits.

Environmental recovery from 137Cs contamination in Japanese coastal waters shown by comparison of temporal distributions with European seas.

We compared the spatiotemporal distributions of 137Cs in the European Baltic Sea (semi-enclosed) and the North and Norwegian Seas (open to the ocean) after the Chernobyl Nuclear Power Plant (CHNPP) accident, with those in Japanese coastal regions, including the waters off Miyagi, Fukushima, and Ibaraki prefectures, open to the western North Pacific, after the Fukushima Nuclear Power Plant accident. The effective half-lives 1-9 years after each accident were shortest (1.6-4.7 y) in Japanese coastal waters, 4.9 y in the North Sea, and 14.4 y in the Baltic Sea, suggesting that decreases in 137Cs concentrations are largely dependent on the local geography, and that the dilution-diffusion effect of seawater was greater in the Japanese coastal waters. The effective half-lives of 137Cs in the surface waters of European seas, based on 30 years of data after the CNPP accident, became longer, ranging from 8.4 to 11.9 y. This may be due to the influence of rivers, and a delay in the decrease in 137Cs levels caused by the small difference in radioactivity concentrations between the seas and diluting waters. These results could contribute to the prediction of contamination levels in Japanese coastal waters in the future.

Temporal variability of 137Cs concentrations in coastal sediments off Fukushima.

Large amounts of radiocesium were released into marine environments following the Fukushima Daiichi Nuclear Power Plant accident in March 2011. Released radiocesium influenced not only marine environment but also marine biota in Fukushima. Since marine biota as fisheries products is important for Japanese market, it is important to assess the distribution of radiocesium in coastal environment off Fukushima for safety concerns of radioactive contamination. Radiocesium concentrations in sediments are important for understanding fishing ground conditions and for proving the safety of fisheries products in Fukushima. In this study, monthly monitoring data collected from May 2011 to March 2020 were analyzed to describe the temporal variability of 137Cs concentrations in coastal sediments off Fukushima (total of 3647 samples from eight lines at depths of 7-125 m off Fukushima, and three sites in Matsukawa-ura Lagoon). The 137Cs concentration in sediment showed a decreasing trend, but our nonlinear model fitting suggested that this rate of decrease had slowed down. Additionally, 137Cs concentrations were up to 4.08 times greater in shallow sampling sites (7, 10, 20 m depth) following heavy rainfall events (before five months vs. after five months), such as typhoons. These observations were consistent with increasing input from particulate 137Cs fluxes from rivers and increasing dissolved 137Cs concentrations in seawater. Finally, our numerical modeling suggested that riverine 137Cs input could maintain 137Cs concentrations in coastal sediment. These results indicate that riverine 137Cs input following heavy rainfall events is the main factor for maintaining 137Cs concentrations in coastal sediments near the Fukushima Daiichi Nuclear Power Plant.

A comparative study of riverine 137Cs dynamics during high-flow events at three contaminated river catchments in Fukushima.

This study presents the temporal variations in riverine 137Cs concentrations and fluxes to the ocean during high-flow events in three coastal river catchments contaminated by the Fukushima Daiichi Nuclear Power Plant accident. River water samples were collected at points downstream in the Niida, Ukedo, and Takase Rivers during three high-flow events that occurred in 2019-2020. Variations in both the dissolved and particulate 137Cs concentrations appeared to reflect the spatial pattern of the 137Cs inventory in the catchments, rather than variations in physico-chemical properties of water and suspended solid. Negative relationships between the 137Cs concentration and δ15N in suspended solid were found in all rivers during the intense rainfall events, suggesting an increased contribution of sediment from forested areas to the elevation of particulate 137Cs concentration. The 137Cs flux ranged from 0.33 to 19 GBq, depending on the rainfall erosivity. The particulate 137Cs fluxes from the Ukedo River were relatively low compared with the other two rivers and were attributed to the effect of the Ogaki Dam reservoir upstream. The percentage of 137Cs desorbed in seawater relative to 137Cs in suspended solids ranged from 2.8% to 6.6% and tended to be higher with a higher fraction of exchangeable 137Cs. The estimated potential release of 137Cs desorbed from suspended solids to the ocean was 0.022-0.57 GBq, and its ratio to the direct flux of dissolved 137Cs was 0.12-6.2. Episodic sampling during high-flow events demonstrated that the particulate 137Cs flux depends on catchment characteristics and controls 137Cs transfer to the ocean.

Factors controlling dissolved 137Cs activities in coastal waters on the eastern and western sides of Honshu, Japan.

The distributions of dissolved 137Cs in river, nearshore, and offshore waters on the east and west coasts of the Japanese island of Honshu were studied in 2018-2021, 7-10 years after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident. On the east side along the north western North Pacific (Fukushima Prefecture), estuarine processes, including desorption from riverine particles and dissolution into pore water from riverine particles that had settled to the seafloor, contributed to the maintenance of high dissolved 137Cs activities in nearshore and offshore waters. A survey and mass-balance calculation in a semi-enclosed estuarine area, the Matsukawa-ura, in the northern part of Fukushima, provided convincing evidence that rivers contributed to the influx of 137Cs to coastal waters. In contrast, the extremely low activities of dissolved and particulate 137Cs in the Tedori River of Ishikawa Prefecture on the western side of Japan along the Japan Sea suggested that inputs of riverine 137Cs made a negligible contribution to the increase of dissolved 137Cs activities in the nearshore and offshore waters. The relatively high dissolved 137Cs activities observed in the offshore waters of the Japan Sea were due to movement of FDNPP-derived 137Cs into the Japan Sea via the Tsushima Warm Current. Mechanisms controlling the distributions of 137Cs activities in coastal waters of the eastern and western sides of Japan therefore differ.

Importance of desorption process from Abukuma River's suspended particles in increasing dissolved 137Cs in coastal water during river-flood caused by typhoons.

Desorption of radiocesium (137Cs) from riverine particles into seawater strongly influences 137Cs concentrations in coastal seawater. This process is important for quantifying the input of radionuclides to marine environments. Here we quantify the particulate 137Cs flux from the Abukuma River, Japan, during typhoon Hagibis and following typhoons in 2019 and estimate the resulting increased dissolved 137Cs levels in coastal seawater. Particulate 137Cs export flux, 1.1 × 1012 Bq, from the Abukuma River during the 4-day period of typhoon Hagibis (12-15 October 2019) equaled two-thirds of the annual flux during 2012-2015, the period of high 137Cs levels following the Fukushima Daiichi Nuclear Power Plant accident. The flux of the desorbed fraction from the Abukuma River during typhoon Hagibis was 0.061-0.12 × 1012Bq, and its daily flux to the surrounding coastal seawater (1.5-3.0 × 1010 Bq/d) was one to two orders of magnitude greater than the estimated input to the coastal seawater during the pre-typhoon period (1.3× 108-1.0 × 109 Bq/d). Simulated results suggest that the massive influx of riverine particles and subsequent desorption of 137Cs increased dissolved 137Cs levels in the coastal seawater by an order of magnitude, from 3.3 mBq/L (pre-typhoon level) to 45-126 mBq/L. This found pathway opens up new scenarios involving radionuclide dynamics in the boundary area of river-sea system.

Suspended Particle-Water Interactions Increase Dissolved 137Cs Activities in the Nearshore Seawater during Typhoon Hagibis.

Distributions of 137Cs in dissolved and particulate phases of the downstream reaches of seven rivers and adjacent nearshore and offshore waters as far as ∼60 km south of the Fukushima Dai-ichi nuclear power plant (FDNPP) were studied during the high-river-flow period (June-September 2019) and during the period of October 2019 after typhoon Hagibis. Dissolved 137Cs activities in nearshore water were higher than those in rivers and offshore waters, and this distribution was more intensified after the typhoon, indicating the desorption of 137Cs from riverine suspended particles in addition to the ongoing release of contaminated water from the FDNPP and re-entry of radiocesium via submarine groundwater discharge. This scenario is also supported by the reduction of distribution coefficient (Kd) from a geometric mean value of 5.5 × 105 L/kg in rivers to 9.8 × 104 L/kg in nearshore water. The occupation of desorbed 137Cs to the dissolved activity of this nuclide in nearshore water was estimated to be 0.7%-20% (median: 9.7%) during the high-river-flow period, increasing to 1.4%-66% (32.3%) after the typhoon, suggesting that the desorption during the flood period such as typhoons further contributes to the increase in dissolved 137Cs levels in nearshore water.

The contribution of 137Cs export flux from the Tone River Japan to the marine environment.

The contribution of 137Cs transport to the marine environment via the Tone River, Japan was investigated. This river has the largest discharge among rivers on the North Pacific side of eastern Japan. The sampling site was located upstream near the river mouth and dissolved and particulate 137Cs in the river water was measured during 2014-2015, three years after the Tokyo Electric Power Corporation Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. Annual fluxes of total (dissolved and particulate) 137Cs with considering desorption of 137Cs from riverine particles by change of salinity from the Tone River were similar in both years (78-107 × 109 Bq/y), indicating that about 0.03-0.06% of the estimated total amount of 137Cs deposited in the catchment (1.9-2.8 × 1014 Bq) was transported to the marine environment each year. Although the annual flux was about one order of magnitude lower than the daily direct discharge into the ocean from the FDNPP (800 × 109 Bq/y) during the corresponding period, continuous monitoring of rivers in the southern coastal area of east Japan on the North Pacific side are needed for the effect of 137Cs release via the rivers in the Kanto area over the long-term.

A 30-year record reveals re-equilibration rates of 137Cs in marine biota after the Fukushima Dai-ichi nuclear power plant accident: Concentration ratios in pre- and post-event conditions.

Concentration ratios (CRs), expressed by dividing 137Cs activity in seawater by that in marine biota (mainly fish), were obtained from the monitoring of 137Cs in coastal areas around Japan between 1984 and 2016. Before the TEPCO Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident (1984-2010), mean CRs of 137Cs, mainly from global fallout (i.e. CRGF), were almost constant for each species throughout the monitoring period, but were different among species, while the values for several species were dependent on their length (i.e. CRGF-SIZE). Thus, CRGF and CRGF-SIZE values for 29 of marketable species are given here as references for conditions where marine biota are in approximate equilibrium (or steady state) with their host water with respect to 137Cs activities in the marine environment. After the FDNPP accident (2011-2016), the impact of the accident has been sustained in eastern Japan waters as indicated by apparent CRs (CRas) which are being used here as indicators of disequilibrium between organisms and their host water. The recession rates of this disequilibrium (the effective CRa half-lives) ranged from 100 to 1100 days. The identified distinct variation was due to the sample locations, even for the same species, because of the change in 137Cs activity concentrations in their host water and diet preference differences. Variation among species, even those captured from the same area, was mainly due to diet differences as well as metabolic-physiological differences in 137Cs retention. Thus, our results from >30 years of systematically monitoring have helped quantify the recession rates of post-FDNPP disequilibrium of 137Cs in biota for assessment of how long term is required from contaminated condition by underlying spatial, inter- and intra-species factors.

Contribution of 137Cs-enriched particles to radiocesium concentrations in seafloor sediment: Reconnaissance experiment.

Autoradiography was used to detect 137Cs-enriched particles in sediment samples. The contributions of 137Cs-enriched particles to 137Cs concentrations in sediment samples ranged from 9% to 64%. These experiments revealed that the variability of 137Cs concentrations was due mainly to the heterogeneous distribution of 137Cs-enriched particles in the samples. Therefore, the heterogeneous distribution of 137Cs-enriched particles is probably one of the main factors responsible for the temporal and spatial variations of 137Cs concentrations in sediment samples.

Radiocesium in the swash zones off the coast of the Japan Sea.

Radiocesium concentrations were measured in seawater and sediment samples collected in the swash zones in Ishikawa and Niigata prefectures, off the coast of Japan Sea opposite to the side where TEPCO Fukushima dai-ichi Nuclear Power Plant (FDNPP) is located in September 2016 and August 2017, five to six years after the accident. Cs-134 in the seawater samples was detected, suggesting the intrusion of FDNPP-derived radiocesium in both swash zones. FDNPP-derived radiocesium was appeared to be transported by the Tsushima Warm Current. In the surface sediments only 137Cs was detected during the sampling period. We could not find out the presence of the FDNPP-derived radiocesium in the corresponding sediment on the swash zones; however, detected radiocesium in those sediments was assumed to be influenced by 137Cs of FDNPP-derived radiocesium little for Ishikawa area and some for Niigata area.

Appearances of Fukushima Daiichi Nuclear Power Plant-Derived 137Cs in Coastal Waters around Japan: Results from Marine Monitoring off Nuclear Power Plants and Facilities, 1983-2016.

Monitoring of 137Cs in seawater in coastal areas around Japan between 1983 and 2016 yielded new insights into the sources and transport of Fukushima Daiichi Nuclear Power Plant (FDNPP)-derived 137Cs, particularly along the west coast of Japan. Before the FDNPP accident (1983-2010), the activity concentrations of 137Cs, mainly from fallout, were decreasing exponentially. Effective 137Cs half-lives in surface seawater ranged from 15.6 to 18.4 yr. After the FDNPP accident (March 2011) 137Cs activity concentrations in seawater off Fukushima and neighboring prefectures immediately increased. Since May/June 2011, 137Cs activity concentrations there have been declining, and they are now approaching preaccident levels. Along the west coast of Japan remote from FDNPP (i.e., the Japan Sea), however, radiocesium activity concentrations started increasing by 2013, with earlier (May/June 2011) increases at some sites due to airborne transport and fallout. The inventory of 137Cs in the Japan Sea (in the main body of the Tsushima Warm Current) in 2016 was calculated to be 0.97 × 1014 Bq, meaning that 0.44 × 1014 Bq of FDNPP-derived 137Cs was added to the estimated global fallout 137Cs inventory in 2016 (0.53 × 1014 Bq). The net increase of 137Cs inventory in the Japan Sea through the addition of FDNPP-derived 137Cs accounts for approximately 0.2% of the total 137Cs flux from the plant to the ocean from the accident.

Temporal variation of cesium isotope concentrations and atom ratios in zooplankton in the Pacific off the east coast of Japan.

After the Fukushima Daiichi Nuclear Power Plant accident in March 2011, concentrations of cesium isotopes (133Cs, 134Cs, and 137Cs) were measured in zooplankton collected in the Pacific off the east coast of Japan from May 2012 to February 2015. The time series of the data exhibited sporadic 137Cs concentration peaks in zooplankton. In addition, the atom ratio of 137Cs/133Cs in zooplankton was consistently high compared to that in ambient seawater throughout the sampling period. These phenomena cannot be explained fully by the bioaccumulation of 137Cs in zooplankton via ambient seawater intake, the inclusion of resuspended sediment in the plankton sample, or the taxonomic composition of the plankton. Autoradiography revealed highly radioactive particles within zooplankton samples, which could be the main factor underlying the sporadic appearance of high 137Cs concentrations in zooplankton as well as the higher ratio of 137Cs/133Cs in zooplankton than in seawater.

The Contribution of Sources to the Sustained Elevated Inventory of (137)Cs in Offshore Waters East of Japan after the Fukushima Dai-ichi Nuclear Power Station Accident.

We have evaluated the contribution of sources of (137)Cs to the inventory of radiocesium in waters (surface area: 6160 km(2), water volume: 753 km(3)) off Fukushima Prefecture and neighboring prefectures from May 2011 to February 2015. A time-series of the inventory of (137)Cs in the offshore waters revealed a clearly decreasing trend from May 2011 (283.4 TBq) to February 2015 (1.89 TBq). The (137)Cs inventory about four years after the accident was approximately twice the background inventory of 1.1 TBq. The magnitudes of the (137)Cs influxes from sources into offshore waters for periods of 182-183 days were estimated from the first period (1 October 2011 to 31 March 2012: 15.3 TBq) to the last period (1 October 2014 to 31 March 2015: 0.41 TBq). We assumed that three sources contributed (137)Cs: continuous direct discharge from the Fukushima Dai-ichi Nuclear Power Station (FNPS) even after the massive discharge in late March 2011, desorption/dissolution from sediments, and fluvial input. Quantification of these sources indicated that the direct discharge from the FNPS is the principal source of (137)Cs to maintain the relatively high inventory in the offshore area.

A new approach to evaluate factors controlling elemental sediment-seawater distribution coefficients (K(d)) in coastal regions, Japan.

In numerical models to simulate the dispersion of anthropogenic radionuclides in the marine environment, the sediment-seawater distribution coefficient (Kd) for various elements is an important parameter. In coastal regions, Kd values are largely dependent on hydrographic conditions and physicochemical characteristics of sediment. Here we report Kd values for 36 elements (Na, Mg, Al, K, Ca, V, Mn, Fe, Co, Ni, Cu, Se, Rb, Sr, Y, Mo, Cd, I, Cs, rare earth elements, Pb, (232)Th and (238)U) in seawater and sediment samples from 19 Japanese coastal regions, and we examine the factors controlling the variability of these Kd values by investigating their relationships to hydrographic conditions and sediment characteristics. There was large variability in Kd values for Al, Mn, Fe, Co, Ni, Cu, Se, Cd, I, Pb and Th. Variations of Kd for Al, Mn, Fe, Co, Pb and Th appear to be controlled by hydrographic conditions. Although Kd values for Ni, Cu, Se, Cd and I depend mainly on grain size, organic matter content, and the concentrations of hydrous oxides/oxides of Fe and Mn in sediments, heterogeneity in the surface characteristics of sediment particles appears to hamper evaluation of the relative importance of these factors. Thus, we report a new approach to evaluate the factors contributing to variability in Kd for an element. By this approach, we concluded that the Kd values for Cu, Se, Cd and I are controlled by grain size and organic matter in sediments, and the Kd value for Ni is dependent on grain size and on hydrous oxides/oxides of Fe and Mn.

Distributions of Pu isotopes in seawater and bottom sediments in the coast of the Japanese archipelago before and soon after the Fukushima Dai-ichi Nuclear Power Station accident.

A radioactivity measurement survey was carried out from 24 April 2008 to 3 June 2011 to determine the levels of plutonium isotopes and (240)Pu/(239)Pu atom ratios in the marine environments off the sites of commercial nuclear power stations around the Japanese islands; the sampling period extended to two months after the Fukushima Dai-ichi Nuclear Power Station accident. In our previous study (Oikawa et al., 2015), data on Pu isotopes and (241)Am in sediments have already been reported. In this study, we report those on Pu isotopes in seawater as well as sediments, and the characteristics of sediments in addition (e.g., ignition loss and biogenic opals). Concentrations of (239+240)Pu in seawater and bottom sediments remained nearly constant at all sampling locations during the survey period. In addition, no regional differences were observed in the (239+240)Pu concentrations in surface waters. Higher (239+240)Pu concentrations were found in bottom waters at deeper sampling locations, but the (240)Pu/(239)Pu atom ratios were nearly constant regardless of the water depth. Higher (239+240)Pu concentrations were also found in bottom sediments at deeper sampling locations, but vice versa for (240)Pu/(239)Pu atom ratios as reported in the previous report. The sediments samples from deeper locations showed the higher percentage of ignition loss as well as the higher content of biogenic opal. There was likely to be some driving force participating in the transfer of Pu isotopes associated with biogenic substances to the deeper seabed. The present survey showed that the accident at the Fukushima Dai-ichi Nuclear Power Station did not contribute much to the inventory of Pu isotopes in the adjacent sea area.

Distribution coefficients (Kd) of strontium and significance of oxides and organic matter in controlling its partitioning in coastal regions of Japan.

The Fukushima Daiichi Nuclear Power Plant accident in March 2011 resulted in the release of large quantities of a long-lived radioactive strontium (i.e. (90)Sr; half-life: 28.8 y) into the coastal areas of Japan. (90)Sr release was dispersed and mixed into the water column, and will eventually be deposited into sediment. Because factors controlling seawater-sediment partitioning in the coastal marine environments are not fully understood, we developed seawater-sediment distribution coefficients, Kd (L/kg), for Sr in coastal regions of Japan by means of sediment-water partitioning experiments. (85)Sr was used as a radiotracer and conditions were designed to mimic the environmental systems of the sampling sites as closely as possible. Experimentally determined Kd values (Kd-ex) varied between 0.3 and 3.3 L/kg (mean, 1.4 L/kg), and the variation in Kd-ex was attributed to the percentage of Sr in the exchangeable fraction in the sediment. Kd-ex values were used, along with the measured concentrations of (88)Sr, a stable naturally occurring Sr isotope in seawater and sediment, to estimate the concentrations of exchangeable Sr in the sediment. Estimates ranged from 2.1 to 24.3 µg/kg, or 1.3-15.7% of the total (88)Sr concentration in the sediment. Significant correlations existed between the estimated concentrations of exchangeable Sr, and the organic matter and the oxide/hydrous oxide contents. When organic contents were greater than 0.38%, Sr binds to organic surface sites more strongly than to the other sites. Results indicate that binding of Sr to the surface of sedimentary particles was influenced by grain size, iron and manganese oxides, and organic matter. Furthermore, the information presented here could be useful to estimate Kd values for anthropogenic (90)Sr in sediment in the coastal marine environment.

Deposition in Chiba prefecture, Japan, of Fukushima Daiichi Nuclear Power Plant fallout.

Radioactivity from the Fukushima Daiichi Nuclear Power Plant (F-1NPP) accident in deposition samples has been monitored at the National Institute of Radiological Sciences (NIRS) in Chiba Prefecture, Japan, located about 220 km south-southwest of the F-1NPP. Sampling was carried out from 15 March 2011, two to three times a day for 10 d and then once a day until 22 April 2011. Gamma-ray spectrometry of fallout deposition samples revealed the presence of (131)I, (132)I, (132)Te, (134)Cs, and (137)Cs. The largest deposition was observed during 7:00-16:00 on 21 March. The estimated total deposition densities at NIRS were 1.40 × 10(5) Bq m(-2) for (131)I, 4.12 × 10(4) Bq m(-2) for (132)Te, 1.45 × 10(4) Bq m(-2) for (134)Cs, and 1.48 × 10(4) Bq m(-2) for (137)Cs (corrected to 11 March 2011). The obtained densities of (134)Cs and (137)Cs were also supported by the accumulated amount of (134)Cs and (137)Cs in soil near the deposition sampling site. For the vertical profile of those radionuclides in soil at NIRS, about 94% of the total deposition was distributed in the top 10 mm depth on 26 April 2011.

Distribution coefficients (K(d)) of stable iodine in estuarine and coastal regions, Japan, and their relationship to salinity and organic carbon in sediments.

The sediment-water distribution coefficient, (K(d)), is one of the most important parameters in radionuclide assessment models. In this study, we determined K ds of stable iodine (I) in estuarine and coastal regions. We studied 16 estuarine and coastal regions of Japan and obtained I data on water and sediments. Data on salinity, pH, dissolved organic carbon and dissolved oxygen in water, and organic carbon (OC) in sediments were also obtained as estuarine variables. Determined (K(d))S of I in the Sagami River estuary decreased along the salinity gradient (salinity range, 0.1-33.8), indicating that salinity is one of the important factors controlling the (K(d)) values; however, when the (K(d)) values were compared among all the estuaries, the difference between minimum and maximum (K(d)) values varied by about two orders of magnitude in a narrow salinity range of 30.0-34.4. A significant correlation between (K(d)) value and OC content in sediments was observed in all the stations with a salinity of ≥ 30 except for stations in the Ishikari and Onga River estuaries. The exceptions are probably due to different sources of the sediments, which are explained by the results of relatively low I/OC ratios in sediments in those two estuaries, compared to the other estuaries. Thus, OC in sediments as well as salinity may be responsible for the variation of (K(d))S of I in the estuarine and coastal regions.

Determination of 232Th in seawater by ICP-MS after preconcentration and separation using a chelating resin.

This article describes an analytical method for the separation, preconcentration and determination of (232)Th in seawater samples at sub-ng/L levels using a NOBIAS CHELATE PA1 resin and a sector field (SF) inductively coupled plasma mass spectrometer (ICP-MS). The resin showed excellent adsorption of (232)Th at a low pH of 2.4 ± 0.4 in a relatively small volume (200 mL) of seawater. (232)Th adsorbed on the resin was easily eluted using 5 mL of 0.8M HNO(3). An enrichment factor of 40 was achieved for (232)Th analysis. Ethylenediamine-tetraacetic acid disodium salt dehydrate (EDTA) was used to investigate the effect of (232)Th-binding organic ligand on the retention of (232)Th on the chelating resin. Results obtained using acidified samples (pH of 2.4 ± 0.4) showed EDTA had no significant effect on (232)Th recovery, indicating that at this low pH, (232)Th was dissociated from the (232)Th-binding organic ligand and quantitatively retained on the NOBIAS CHELATE PA1 resin. The developed analytical method was characterized by a separation and preconcentration taking approximately 4h and a low detection limit of 0.0038 ng/L for (232)Th, and was successfully applied to the determination of (232)Th in seawater samples collected from coastal areas, Japan.