Horizontal distribution of surface microplastic concentrations and water-column microplastic inventories in the Chukchi Sea, western Arctic Ocean.

The recent influx of microplastics into the Arctic Ocean may increase environmental stress on the western Arctic marine ecosystem, which is experiencing significant sea-ice loss due to global warming. Quantitative data on microplastics in the western Arctic Ocean are very limited, and the microplastic budget of the water column is completely unknown. To fill in gaps in our knowledge of Arctic microplastics, we observed surface concentrations (number of particles per unit volume of seawater) of meso- and microplastics using a neuston net, and we observed wind speeds and significant wave heights in the Chukchi Sea, Bering Strait, and Bering Sea. From these observations, we estimated the total number (particle inventory) and mass (mass inventory) of microplastics in the entire water column by taking into account the effect of vertical mixing. The particle inventory of microplastics in the Chukchi Sea ranged from 0 to 18,815 pieces km-2 with a mean and standard deviation of 5236 ± 6127 pieces km-2. The mass inventory ranged from 0 to 445 g km-2 with a mean and standard deviation of 124 ± 145 g km-2. Mean particle inventories for the Chukchi Sea were one-thirtieth of those for the Arctic Ocean on the Atlantic side and less than one-tenth of the average for the global ocean, suggesting that the Chukchi Sea is less polluted. However, the annual flux of microplastics from the Pacific Ocean into the Chukchi Sea, estimated from microplastic concentrations in the Bering Strait, was about 5.5 times greater than the total amount of microplastic in the entire Chukchi Sea water. This suggests that microplastic inflows from the Pacific Ocean are accumulating in large amounts in reservoirs other than the Chukchi Sea water (e.g., sea ice and seafloor sediments) or in the downstream regions of the Pacific-origin water.

Cesium-137 and 137Cs/133Cs atom ratios in marine zooplankton off the east coast of Japan during 2012-2020 following the Fukushima Dai-ichi nuclear power plant accident.

We measured the concentrations of cesium isotopes (133Cs, 134Cs, and 137Cs) in zooplankton samples collected in waters off the east coast of Japan from May 2015 to June 2020. By combining these data with those obtained previously from May 2012 to February 2015, we evaluated the long-term impacts of the Fukushima Dai-ichi Nuclear Power Plant accident on marine zooplankton. Relatively high 137Cs concentrations in zooplankton, exceeding 10 Bq/kg-dry weight, were sporadically observed until June 2016, regardless of year or station. After May-June 2017, 137Cs concentrations decreased to below 1 Bq/kg-dry at most stations, and by May 2020, concentrations were below 0.5 Bq/kg-dry except those off Fukushima Prefecture. Since the accident, the 137Cs/133Cs atom ratios of zooplankton samples were higher than those of ambient seawater until 2019, but in May-June 2020 the ratios matched those of seawater except off Fukushima Prefecture. Highly radioactive particles were not detected in zooplankton samples by autoradiography using imaging plates after May-June 2017, although they were before. Therefore, the persistence of elevated 137Cs/133Cs ratios in zooplankton relative to seawater for nine years after the accident was probably due to the incorporation of highly radioactive particles (cesium-bearing particles or clay-mineral aggregates with highly adsorbed radiocesium) onto/into zooplankton for several years after the accident. However, since at least May-June 2017, these elevated ratios have likely been caused by small highly radioactive particles (or larger particles disaggregated into small pieces) entering the ocean from land via rivers or directly discharged from the Fukushima Nuclear Power Plant. Microplastics enriched with radiocesium with higher 137Cs/133Cs ratios than seawater may have also contributed 137Cs to the zooplankton.

Occurrence of highly radioactive microparticles in the seafloor sediment from the pacific coast 35 km northeast of the Fukushima Daiichi nuclear power plant.

To understand the properties and significance of highly radioactive particles in the marine environment, we have examined seafloor sediment with a radioactivity of ∼1200 Bq/kg (dry weight; after decay correction to March 2011) collected 35 km northeast of the Fukushima Daiichi Nuclear Power Plant (FDNPP). Among the 697 highly radioactive particles separated from the sediment, two particles, D1-MAX and D1-MID, had a total Cs radioactivity of ∼56 and 0.67 Bq (after decay correction to March 2011), respectively. These particles were characterized with a variety of electron microscopic techniques, including transmission electron microscopy. The 134Cs/137Cs radioactivity ratio of D1-MAX, 1.04, was comparable to that calculated for Unit 2 or 3. D1-MAX consisted mainly of a Cs-rich microparticle (CsMP) with a silica glass matrix. The data clearly suggested that D1-MAX resulted from a molten core-concrete interaction during meltdowns. In contrast, D1-MID was an aggregate of plagioclase, quartz, anatase, and Fe-oxide nanoparticles as well as clay minerals, which had adsorbed soluble Cs. D1-MID was likely a terrestrial particle that had been transported by wind and/or ocean currents to a site 35 km from the FDNPP. The radioactive fractions of D1-MAX and D1-MID were 15% and 0.36%, respectively, of the total radioactivity in the bulk sediment. These highly radioactive particles have a great impact on the movement of radioactive Cs in the marine environment by carrying condensed Cs radioactivity with various colloidal and desorption properties depending on the host phase.

Temporal variation of iodine-129 concentrations in kelps (Saccharina) from coastal waters off northern Japan.

Concentrations of 129I and 127I in kelps (Saccharina) collected from coastal waters off northern Japan were monitored from 2007 to 2019. During the 2007-2008 test operation of the Rokkasho nuclear fuel reprocessing plant, 129I discharge from the plant increased, and the 129I concentration and 129I/127I atom ratio in the kelps reached maxima of 42 µBq/g-dry and 264 × 10-11, respectively. By 2009, both had decreased by one order of magnitude. After the Fukushima Dai-ichi Nuclear Power Plant accident in 2011, the 129I concentration and 129I/127I atom ratio in the kelps increased to 2.24 µBq/g-dry and 11.6 × 10-11, respectively. After 2012, the ratio in kelps decreased to (2.1-8.9) × 10-11, which is almost the same as the seawater value off Aomori Prefecture before the test operation. The 129I/127I atom ratio in kelps thus represents the ambient seawater ratio during the growth period of the kelps.

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.

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.