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Journal Articles

Seven-year temporal variation of cesium-137 discharge inventory from the port of Fukushima Dai-ichi Nuclear Power Plant; Continuous monthly estimation of cesium-137 discharge in the period from April 2011 to June 2018

Machida, Masahiko; Yamada, Susumu; Iwata, Ayako; Otosaka, Shigeyoshi; Kobayashi, Takuya; Watanabe, Masahisa; Funasaka, Hideyuki; Morita, Takami*

Nippon Genshiryoku Gakkai Wabun Rombunshi, 18(4), p.226 - 236, 2019/12

After direct discharges of highly-contaminated water from Unit 2 and 3 in Fukushima Daiichi Nuclear Power Plant (1F) in April to May 2011, Kanda suggested that relatively small run-off of radionuclides from 1F port into Fukushima coastal region has subsequently continued by using his estimation scheme. However, the estimation period was limited until September 2012, and there has been no report on the issue since the work. Therefore, this paper focuses on discharge inventory from 1F port until June 2018. In the missing period, the central government and Tokyo Electric Power Company Holdings have done continuous efforts to stop the discharge, and consequently sea water concentration inside 1F port has diminished gradually. We show monthly discharge inventory of Cs-137 until June 2018 by two schemes, i.e., Kanda's scheme partially improved by authors and more sophisticated one using Voronoi tessellation reflecting the increment of the number of monitoring points inside 1F port. The results show that the former always presents overestimated results compared to the latter but the ratio of former to latter is less than one order. Based on these results, we evaluate impact of discharge inventory from 1F port into the coastal area and radiation does via fish digestion.

Journal Articles

Repeatability and reproducibility of measurements of low dissolved radiocesium concentrations in freshwater using different pre-concentration methods

Kurihara, Momo*; Yasutaka, Tetsuo*; Aono, Tatsuo*; Ashikawa, Nobuo*; Ebina, Hiroyuki*; Iijima, Takeshi*; Ishimaru, Kei*; Kanai, Ramon*; Karube, Jinichi*; Konnai, Yae*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 322(2), p.477 - 485, 2019/11

 Times Cited Count:0 Percentile:100(Chemistry, Analytical)

We assessed the repeatability and reproducibility of methods for determining low dissolved radiocesium concentrations in freshwater in Fukushima. Twenty-one laboratories pre-concentrated three of 10 L samples by five different pre-concentration methods (prussian-blue-impregnated filter cartridges, coprecipitation with ammonium phosphomolybdate, evaporation, solid-phase extraction disks, and ion-exchange resin columns), and activity of radiocesium was measured. The z-scores for all of the $$^{137}$$Cs results were within $$pm$$2, indicating that the methods were accurate. The relative standard deviations (RSDs) indicating the variability in the results from different laboratories were larger than the RSDs indicating the variability in the results from each separate laboratory.

Journal Articles

Penetration of $$^{129}$$I released from Fukushima Daiichi Nuclear Power Plant accident in the western North Pacific Ocean

Suzuki, Takashi; Otosaka, Shigeyoshi; Kuwabara, Jun; Kawamura, Hideyuki; Kobayashi, Takuya

JAEA-Conf 2018-002, p.103 - 106, 2019/02

To investigate the dynamics of radionuclides in the ocean released by the accident at Fukushima Daiichi Nuclear Power Plant (1F), vertical distributions of $$^{129}$$ I at three stations in the western North Pacific was revealed. The 1F accident-derived $$^{129}$$ I existed within the mixed layer at 3 stations. The maximum layer of the 1F accident-derived $$^{129}$$ I existed at the depth of 370 m - 470 m at the most southern station. Considering the dissolved oxygen concentration and the current velocity arround the station, the maximum layer of the 1F accident-derived $$^{129}$$ I would be fromed that $$^{129}$$I which existed in the surface seawater at other area of observation point was carried to the depth of 370 m - 470 m by the fast downward flow.

Journal Articles

Distribution and fate of $$^{129}$$I in the seabed sediment off Fukushima

Otosaka, Shigeyoshi; Sato, Yuhi*; Suzuki, Takashi; Kuwabara, Jun; Nakanishi, Takahiro

Journal of Environmental Radioactivity, 192, p.208 - 218, 2018/12

 Times Cited Count:4 Percentile:60.68(Environmental Sciences)

From August 2011 to October 2013, the concentration of iodine-129 ($$^{129}$$I) in the seabed sediment collected from 26 stations located within 160 km from the Fukushima Daiichi Nuclear Power Plant was estimated. The concentrations of $$^{129}$$I in seabed sediment off Fukushima in 2011 ranged between 0.02 and 0.45 mBq/kg. Although iodine is a biophilic element, the accident-derived radioiodine negligibly affects the benthic ecosystem. Until October 2013, a slightly increased activity of $$^{129}$$I in the surface sediment in the shelf-edge region (bottom depth: 200-400 m) was observed. The increase of the $$^{129}$$I concentrations in the shelf-edge sediments was affected by the (1) transport of $$^{129}$$I-bound particles from the land through rivers and (2) re-deposition of $$^{129}$$I desorbed from the contaminated coastal sediment to the shelf-edge sediments, which were considered to be dominant processes.

Journal Articles

Vertical distribution of $$^{129}$$I released from the Fukushima Daiichi Nuclear Power Plant in the Kuroshio and Oyashio current areas

Suzuki, Takashi; Otosaka, Shigeyoshi; Kuwabara, Jun; Kawamura, Hideyuki; Kobayashi, Takuya

Marine Chemistry, 204, p.163 - 171, 2018/08

 Times Cited Count:0 Percentile:100(Chemistry, Multidisciplinary)

To investigate the penetration of radionuclides released from Fukushima Daiichi Nuclear Power Plant (FDNPP), depth profiles were revealed at Kuroshio current, transition, and Oyashio current areas. The FDNPP-derived $$^{129}$$I was found in surface layer at Oyashio current and transition areas and in sub-surface layer at Kuroshio current area. Moreover, it was found that the FDNPP-derived $$^{129}$$I/$$^{134}$$Cs ratios in the Oyashio current and transition areas were higher than that in the FDNPP reactor. The higher FDNPP-derived $$^{129}$$I/$$^{134}$$Cs ratios suggest three potential mechanisms for the migration of radionuclides in the environment: (1) radioiodine was released more easily than radiocesium by the FDNPP accident, (2) $$^{129}$$I was supplied from the atmosphere by re-emitted $$^{129}$$I from contaminated areas around Fukushima, (3) leaked water that removed radiocesium reached the sampling stations. The FDNPP-derived $$^{129}$$I in sub-surface layer would be transported by the meander of the Kuroshio Extension current.

Journal Articles

$$delta^{13}$$C and $$delta^{15}$$N values of sediment-trap particles in the Japan and Yamato Basins and comparison with the core-top values in the East/Japan Sea

Khim, B.-K.*; Otosaka, Shigeyoshi; Park, K.-A.*; Noriki, Shinichiro*

Ocean Science Journal, 53(1), p.17 - 29, 2018/03

 Times Cited Count:1 Percentile:79(Marine & Freshwater Biology)

Distribution of carbon and nitrogen stable isotope ratios ($$delta$$$$^{13}$$C, $$delta$$$$^{15}$$N) in sinking particles collected in four stations in the Japan Sea was summarized. The $$delta$$$$^{13}$$C and $$delta$$$$^{15}$$N values in the sinking particles showed a clear seasonal variation, which agreed well with the variation in the chlorophyll a concentration in the surface seawater and in the sinking flux of biogenic particles. In particular, during the highly productive season of phytoplankton, a remarkable isotopic fractionation of $$delta$$$$^{13}$$N was found in the sinking particles, and it was inferred that the fractionation indicates the degree of nitrogen uptake by diatoms in the surface layer. These results are helpful information for linking the phenomenon in the ocean surface and the isotopic information recorded in the seafloor.

Journal Articles

Factors controlling $$^{134}$$Cs activity concentrations in sediment collected off the coast of Fukushima Prefecture in 2013-2015

Fukuda, Miho*; Aono, Tatsuo*; Yamazaki, Shinnosuke*; Ishimaru, Takashi*; Kanda, Jota*; Nishikawa, Jun*; Otosaka, Shigeyoshi

Geochemical Journal, 52(2), p.201 - 209, 2018/00

 Times Cited Count:2 Percentile:63.06(Geochemistry & Geophysics)

To elucidate recent activity levels and the behavior of radiocesium in the coast off Fukushima Prefecture, lateral and vertical distributions of $$^{134}$$Cs in sediment were observed in 2013-2015 at 12 monitoring stations. At stations around the water depth of 100 m, relatively higher $$^{134}$$Cs activities were observed from surface sedimentary layer (0-3 cm). In these stations, sediments had high content of silt to clay particles and organic matter. The high $$^{134}$$Cs activities in the surface sediments were attributed to accumulation of highly mobile sediment particles. In October 2014, at some coastal stations, sharp peaks of $$^{134}$$Cs activities were observed in the subsurface (5-16 cm) sediments, whereas such broad peaks were not found in October 2015. These results suggest that the $$^{134}$$Cs activities in sediment had largely changed by lateral transport and re-sedimentation on the surface, as well as sediment mixing in the middle-layers.

Journal Articles

Challenges for enhancing Fukushima environmental resilience, 7; Behavior and abundance of radiocesium in the coastal area off Fukushima

Otosaka, Shigeyoshi; Kobayashi, Takuya; Machida, Masahiko

Nippon Genshiryoku Gakkai-Shi, 59(11), p.659 - 663, 2017/11

It is estimated that about 70% of radiocesium released to the environment by the Fukushima Daiichi nuclear accident was carried to the ocean. In addition to monitoring surveys by the government, oceanographic research by many institutions has revealed the distribution and behavior of the accident-derived radiocesium in the ocean. Numerical simulations are efficiently used in such oceanographic investigations, and further improvements are being made based on findings newly obtained after the accident. In this paper, we review the abundance and behavior of radiocesium in the coastal area of Fukushima, deepen the scientific understanding of the current situation of environmental restoration, and explain the issues to be addressed in the future.

Journal Articles

Processes affecting long-term changes in $$^{137}$$Cs concentration in surface sediments off Fukushima

Otosaka, Shigeyoshi

Journal of Oceanography, 73(5), p.559 - 570, 2017/10


 Times Cited Count:9 Percentile:22.59(Oceanography)

Based on monitoring data from 71 stations off the coast of Fukushima, Miyagi and Ibaraki Prefectures, changing tendencies of $$^{137}$$Cs concentration in surface (0-10 cm) sediment are analyzed, and primary processes affecting the temporal changes are determined. In the coastal region (water depth $$<$$ 100m), between 2011 and 2015, concentrations of $$^{137}$$Cs in the surface sediment decreased at the rate of 27% per year in average. Such a remarkable temporal change in the $$^{137}$$Cs concentration of sedimentary radiocesium was not observed in the offshore regions. By applying observed data of vertical distribution of sedimentary $$^{137}$$Cs into a pulse input sediment mixing model, it was estimated that more than a half of the decreasing effect was explained by vertical mixing of $$^{137}$$Cs-bound surface sediment with less-contaminated sediment in the deeper layers.

Journal Articles

Preface "Radionuclides in coastal sediments after the accident of Fukushima Daiichi Nuclear Power Plant; Distribution, dynamics and fate"

Nagao, Seiya*; Otosaka, Shigeyoshi; Kaeriyama, Hideki*

Journal of Oceanography, 73(5), P. 527, 2017/10

 Times Cited Count:1 Percentile:44.38(Oceanography)

More than five years have passed since the accident at the Fukushima Daiichi Nuclear Power Plant, and many investigations have been carried out in the marine environment. Regarding the radiocesium concentration in seabed sediment, from May 2011, monitoring survey is continuing mainly in the coastal areas of Miyagi, Fukushima, Ibaraki and Chiba prefectures. However, due to its heterogeneity, the difficulty of observation, etc., the assessment of the influence of the accident-derived radionuclides on seabed sediments and the benthic ecosystem is delayed compared to other environmental investigations. As the Guest Editors, the authors set up a special section in "Journal of Oceanography", including four papers arguing about factors affecting the temporal change of the radiocesium concentrations in estuarine, coastal and offshore sediments. This preface shows the planning intention of the special issue, and also outlines the contents.

Journal Articles

Dissolved radiocaesium in seawater off the coast of Fukushima during 2013-2015

Fukuda, Miho*; Aono, Tatsuo*; Yamazaki, Shinnosuke*; Nishikawa, Jun*; Otosaka, Shigeyoshi; Ishimaru, Takashi*; Kanda, Jota*

Journal of Radioanalytical and Nuclear Chemistry, 311(2), p.1479 - 1484, 2017/02

 Times Cited Count:3 Percentile:45.4(Chemistry, Analytical)

In order to investigate processes affecting distribution of radiocaesium in seawater in the adjacent region of Fukushima Daiichi Nuclear Power Plant (FDNPP), relationships between $$^{137}$$Cs activity in seawater and physical properties of seawater (salinity, temperature, and potential density) were observed in seven stations within 10 km radius from the FDNPP. As a whole, $$^{137}$$Cs concentrations in seawater were higher in the vicinity of the FDNPP, and were negatively correlated with potential density. From these results, it can be considered that river water discharge or export of seawater from the FDNPP's harbor has affected the higher activity levels of $$^{137}$$Cs in seawater. It was also observed that the $$^{137}$$Cs-elevated seawater can be advected to the 20$$sim$$50 m depths.

Journal Articles

Year-round variations in the fluvial transport load of particulate $$^{137}$$Cs in a forested catchment affected by the Fukushima Daiichi Nuclear Power Plant accident

Matsunaga, Takeshi; Nakanishi, Takahiro; Atarashi-Andoh, Mariko; Takeuchi, Erina; Muto, Kotomi; Tsuzuki, Katsunori; Nishimura, Shusaku; Koarashi, Jun; Otosaka, Shigeyoshi; Sato, Tsutomu*; et al.

Journal of Radioanalytical and Nuclear Chemistry, 310(2), p.679 - 693, 2016/11


 Times Cited Count:5 Percentile:34.28(Chemistry, Analytical)

Particulate $$^{137}$$Cs in stream water was collected continuously for two years in order to assess the long-term trend of the $$^{137}$$Cs discharge from the forest environment. Sampling was conducted from December 2011 to December 2013 in a mountainous stream, which received the $$^{137}$$Cs from the Fukushima Daiichi Nuclear Power Plant accident. A seasonal increase in fluvial transport load of particulate $$^{137}$$Cs associated with suspended solids (SS) was observed in August and September when rainfall was abundant. The particulate $$^{137}$$Cs concentration decreased at a faster rate than the rate due to radioactive decay. This decrease might be resulted from redistribution of the easily eroded and polluted soil surface due to heavy rain events such as typhoons. These findings indicate that the particulate $$^{137}$$Cs load was subject to the inter-annual variations in rainfalls, and decreased gradually over a long period of time due to a decrease in $$^{137}$$Cs concentration in SS.

Journal Articles

Resuspension and lateral transport of seafloor sediment contaminated with artificial radionuclides derived from Fukushima Daiichi Nuclear Power Plant accident

Honda, Makio*; Otosaka, Shigeyoshi

Nippon Genshiryoku Gakkai-Shi, 58(4), p.225 - 228, 2016/04

Transport processes of particulate radiocesium obtained from a three year time-series sediment trap experiments at a site 115 km southeast of Fukushima Daiichi Nuclear Power Plant off Fukushima are expounded. Results show a high fraction of lithogenic material in sinking particles, suggesting a lateral source of sediments. In particular, we found that accident-derived radiocesium associate with slope and shelf sediments were resuspended and transported laterally to the offshore regions in typhoon seasons in 2013. Continuous observation of such transport processes of particulate radiocesium near the seabed would be significant for better understanding of the fate of accident-derived radiocesium.

Journal Articles

Tracking the fate of particle associated Fukushima Daiichi cesium in the ocean off Japan

Buesseler, K. O.*; German, C. R.*; Honda, Makio*; Otosaka, Shigeyoshi; Black, E. E.*; Kawakami, Hajime*; Manganini, S. M.*; Pike, S.*

Environmental Science & Technology, 49(16), p.9807 - 9816, 2015/08

 Times Cited Count:11 Percentile:47.29(Engineering, Environmental)

A three year time-series of particle fluxes is presented from sediment traps deployed at 500 and 1000 m at a site 115 km southeast of Fukushima Daiichi Nuclear Power Plant (FDNPP). Results show a high fraction of lithogenic material, suggesting a lateral source of sediments. The accident-derived radiocesium were enhanced in flux peaks that, given variations in trap $$^{137}$$Cs/$$^{210}$$Pb ratios, are characteristic of material derived from shelf and slope sediments found from $$<$$ 120 to $$>$$ 500 m. The fluxes of radiocesium are an order of magnitude higher than a previously reported for the trap located 100 km due east of FDNPP. We attribute the large difference due to the position of our trap under the southeasterly currents that carry contaminated waters and resuspended sediments in to the Pacific. These higher sedimentary fluxes of radiocesium to the offshore are still small relative to the inventory of radiocesium currently buried nearshore.

Journal Articles

A Passive collection system for whole size fractions in river suspended solids

Matsunaga, Takeshi; Nakanishi, Takahiro; Atarashi-Andoh, Mariko; Takeuchi, Erina; Tsuzuki, Katsunori; Nishimura, Shusaku; Koarashi, Jun; Otosaka, Shigeyoshi; Sato, Tsutomu*; Nagao, Seiya*

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1291 - 1295, 2015/02

 Times Cited Count:3 Percentile:61.2(Chemistry, Analytical)

An innovative, yet simple method for the passive collection of radioactive materials in river water has been developed and validated. The method employes large filter vessels, containing multiple cartridge filters. River water is led to the system naturally using a drop of the riverbed by hose from upstream. This method makes long-term, unmanned monitoring possible. In addition to regular radioactivity analyses, this method provides an opportunity for the characterization of suspended materials based on its ample collection quantities (more than several tens of grams). This method may also be applicable to sediment-bound chemicals.

Journal Articles

Vertical and lateral transport of particulate radiocesium off Fukushima

Otosaka, Shigeyoshi; Nakanishi, Takahiro; Suzuki, Takashi; Sato, Yuhi; Narita, Hisashi*

Environmental Science & Technology, 48(21), p.12595 - 12602, 2014/11

 Times Cited Count:13 Percentile:46.61(Engineering, Environmental)

From August 2011 to July 2013, a sediment trap was deployed at 100 km east of the Fukushima Daiichi Nuclear Power Plant and sinking particles were collected. Sinking flux of $$^{137}$$Cs decreased over time with seasonal fluctuation. The $$^{137}$$Cs fluxes were mainly affected by two principal modes. One was a rapid sinking of radiocesium-bound particles (moderate mode). This mode was dominant especially in the early post-accident stage, and was presumed to establish the distribution of radiocesium in the offshore seabed. Another was the secondary transport of particles attributed to turbulence near the seabed and was observed in winter (turbulence mode). Although the latter process would not drastically change the distribution of sedimentary radiocesium, attention should be paid as this key process redistributing the accident-derived radiocesium may cumulatively affect the long-term distribution.

Journal Articles

Speciation of iodine isotopes inside and outside of a contaminant plume at the Savannah River Site

Schwehr, K. A.*; Otosaka, Shigeyoshi; Merchel, S.*; Kaplan, D. I.*; Zhang, S.*; Xu, C.*; Li, H.-P.*; Ho, Y.-F.*; Yeager, C. M.*; Santschi, P. H.*; et al.

Science of the Total Environment, 497-498, p.671 - 678, 2014/11

 Times Cited Count:9 Percentile:63.1(Environmental Sciences)

A new, accurate and simple pH-dependent solvent extraction method combined with accelerator mass spectrometry (AMS) measurement for $$^{129}$$I/$$^{127}$$I isotopes and iodine speciation (iodide, iodate, and organo-I) quantification in liquids of any ionic strength has been developed. We then validated the AMS method for activity concentration measurements with a recently developed gas chromatography mass spectrometry method for $$^{129}$$I concentrations of 1 Bq/L or higher. This technique was applied to $$^{129}$$I-contaminated groundwater from the Savannah River Site, USA, and demonstrated changes of $$^{129}$$I and $$^{127}$$I concentrations and speciation along a pH, redox potential, and organic carbon gradient. The data suggest that $$^{129}$$I/$$^{127}$$I and species distribution is strongly pH dependent. The new method can now be applied to a wide range of chemically-diverse aquatic systems, including uncontaminated environments.

Journal Articles

Radiocesium derived from the Fukushima Daiichi Nuclear Power Plant accident in seabed sediments; Initial deposition and inventories

Otosaka, Shigeyoshi; Kato, Yoshihisa*

Environmental Science; Processes & Impacts, 16(5), p.978 - 990, 2014/05

 Times Cited Count:26 Percentile:19.16(Chemistry, Analytical)

Since the accident of Fukushima Daiichi Nuclear Power Plant (1FNPP), significant levels of anthropogenic radionuclides have been detected from seabed sediments off the east coast of Japan. In this paper, the approximate amount of accident-derived radiocesium in seabed sediments off Fukushima, Miyagi and Ibaraki prefectures was estimated. As of October 2011, the total amount of sedimentary $$^{134}$$Cs was 0.20$$pm$$0.05 PBq (decay corrected to March 11, 2011) and about 95% of the radiocesium was accumulated in the regions shallower than 200 m depths. The large inventory in the coastal sediments was attributed to effective adsorption of dissolved radiocesium onto sediments. Although rivers are also an important source to supply radiocesium to the coastal regions, the potential was relatively lower than that of the above-mentioned process at least in the early stage, within half a year, after the accident.

Journal Articles

Determination of total iodine concentration in aquatic environments using cathodic stripping voltammetry combined with sodium hypochlorite (NaClO) oxidation

Sato, Yuhi; Otosaka, Shigeyoshi; Suzuki, Takashi

Journal of Water and Environment Technology (Internet), 12(2), p.201 - 210, 2014/04

An easy and fast method for determination of total iodine in environmental samples by cathodic stripping voltammetry combined with NaClO oxidation has been developed. Adequate conditions for NaClO oxidation of 40-50$$^{circ}$$C over 2 h were determined, using three representative environmental samples (reference soil, seabed sediment, seaweed). By analyzing a mixture of thyroxin and a reference soil material, we obtained an overall recovery of more than 97% for total iodine in the concentration range of 1-7 $$mu$$mol g$$^{-1}$$. This method was compared with alkaline extraction and combustion methods for solid and aqueous environmental samples. Alkaline extraction exhibited lower recovery of iodine compared with the NaClO oxidation method, indicating insufficient extraction and/or interference on determination. Combustion method also showed lower iodine recovery for some samples, probably due to a trapping efficiency and incomplete combustion of organic matter.

Journal Articles

Sedimentation and remobilization of radiocesium in the coastal area of Ibaraki, 70 km south of the Fukushima Dai-ichi Nuclear Power Plant

Otosaka, Shigeyoshi; Kobayashi, Takuya

Environmental Monitoring and Assessment, 185(7), p.5419 - 5433, 2013/07


 Times Cited Count:54 Percentile:9.52(Environmental Sciences)

From a time-series observation at 9 stations off the coast of Ibaraki, the following transport processes of sedimentary radiocesium can be inferred. (1) Major distributional pattern of the 1FNPP-derived radiocesium in coastal sediments was configurated within half a year after the accident. (2) Larger inventories of sedimentary radiocesium in the shallow region attribute to the higher contact probability of dissolved radiocesium with sediment. (3) Most of radiocesium in the coastal sediments is incorporated into lithogenic fractions, and the incorporation is almost irreversible. (4) Radiocesium is selectively accumulated in the finer-grained sediments. (5) In the study area, as of January 2012, riverine input of suspended particulate matter can be regarded as a minor process to accumulate radiocesium in the coastal sediments. Nevertheless, the relative contribution would increase years later.

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