Distribution and Evolution of Fukushima Dai-ichi derived 137Cs, 90Sr, and 129I in Surface Seawater off the Coast of Japan.

The Fukushima Dai-ichi Nuclear Power Plants (FDNPPs) accident in 2011 led to an unprecedented release of radionuclides into the environment. Particularly important are 90Sr and 137Cs due to their known health detriments and long half-lives (T1/2 ≈ 30 y) relative to ecological systems. These radionuclides can be combined with the longer-lived 129I (T1/2 = 15.7 My) to trace hydrologic, atmospheric, oceanic, and geochemical processes. This study seeks to evaluate 137Cs, 90Sr, and 129I concentrations in seawater off the coast of Japan, reconcile the sources of contaminated waters, and assess the application of 137Cs/90Sr, 129I/137Cs, and 129I/90Sr as oceanic tracers. We present new data from October 2015 and November 2016 off the coast of Japan, with observed concentrations reaching up to 198 ± 4 Bq·m-3 for 137Cs, 9.1 ± 0.7 Bq·m-3 for 90Sr, and (114 ± 2) × 10-5 Bq·m-3 for 129I. The utilization of activity ratios suggests a variety of sources, including sporadic and independent releases of radiocontaminants. Though overall concentrations are decreasing, concentrations are still elevated compared to pre-accident levels. In addition, Japan's Environment Minister has suggested that stored water from the FDNPPs may be released into the environment and thus continued efforts to understand the fate and distribution of these radionuclides is warranted.

Lingering radioactivity at the Bikini and Enewetak Atolls.

We made an assessment of the levels of radionuclides in the ocean waters, seafloor and groundwater at Bikini and Enewetak Atolls where the US conducted nuclear weapons tests in the 1940's and 50's. This included the first estimates of submarine groundwater discharge (SGD) derived from radium isotopes that can be used here to calculate radionuclide fluxes in to the lagoon waters. While there is significant variability between sites and sample types, levels of plutonium (239,240Pu) remain several orders of magnitude higher in lagoon seawater and sediments than what is found in rest of the world's oceans. In contrast, levels of cesium-137 (137Cs) while relatively elevated in brackish groundwater are only slightly higher in the lagoon water relative to North Pacific surface waters. Of special interest was the Runit dome, a nuclear waste repository created in the 1970's within the Enewetak Atoll. Low seawater ratios of 240Pu/239Pu suggest that this area is the source of about half of the Pu in the Enewetak lagoon water column, yet radium isotopes suggest that SGD from below the dome is not a significant Pu source. SGD fluxes of Pu and Cs at Bikini were also relatively low. Thus radioactivity associated with seafloor sediments remains the largest source and long term repository for radioactive contamination. Overall, Bikini and Enewetak Atolls are an ongoing source of Pu and Cs to the North Pacific, but at annual rates that are orders of magnitude smaller than delivered via close-in fallout to the same area.

Reassessment of (90)Sr, (137)Cs, and (134)Cs in the Coast off Japan Derived from the Fukushima Dai-ichi Nuclear Accident.

The years following the Fukushima Dai-ichi nuclear power plant (FDNPP) accident, the distribution of (90)Sr in seawater in the coast off Japan has received limited attention. However, (90)Sr is a major contaminant in waters accumulated within the nuclear facility and in the storage tanks. Seawater samples collected off the FDNPP in September 2013 showed radioactive levels significantly higher than pre-Fukushima levels within 6 km off the FDNPP. These samples, with up to 8.9 ± 0.4 Bq·m(-3) for (90)Sr, 124 ± 3 Bq·m(-3) for (137)Cs, and 54 ± 1 Bq·m(-3) for (134)Cs, appear to be influenced by ongoing releases from the FDNPP, with a characteristic (137)Cs/(90)Sr activity ratio of 3.5 ± 0.2. Beach surface water and groundwater collected in Sendai Bay had (137)Cs concentrations of up to 43 ± 1 Bq·m(-3), while (90)Sr was close to pre-Fukushima levels (1-2 Bq·m(-3)). These samples appear to be influenced by freshwater inputs carrying a (137)Cs/(90)Sr activity ratio closer to that of the FDNPP fallout deposited on land in the spring of 2011. Ongoing inputs of (90)Sr from FDNPP releases would be on the order of 2.3-8.5 GBq·d(-1) in September 2013, likely exceeding river inputs by 2-3 orders of magnitude. These results strongly suggest that a continuous surveillance of artificial radionuclides in the Pacific Ocean is still required.

Tracking the Fate of Particle Associated Fukushima Daiichi Cesium in the Ocean off Japan.

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 and mass flux peaks that do not align between the trap depths, suggesting a lateral source of sediments. Fukushima cesium-137 and cesium-134 were enhanced in flux peaks that, given variations in trap (137)Cs/(210)Pbex ratios, are characteristic of material derived from shelf and slope sediments found from <120 to >500 m. These lateral flux peaks are possibly triggered by passing typhoons. The Cs fluxes are an order of magnitude higher than were previously reported for the trap located 100 km due east of FDNPP. We attribute this large difference to the position of our trap under the southeasterly currents that carry contaminated waters and resuspended sediments away from FDNPP and into the Pacific. These higher Cs sedimentary fluxes offshore are still small relative to the inventory of Cs currently buried nearshore. Consequently, we do not expect them to effect any rapid decrease in Cs levels for the coastal sediments near FDNPP that have been linked to enhanced Cs in demersal fish.

Fukushima-derived radionuclides in the ocean and biota off Japan.

The Tohoku earthquake and tsunami of March 11, 2011, resulted in unprecedented radioactivity releases from the Fukushima Dai-ichi nuclear power plants to the Northwest Pacific Ocean. Results are presented here from an international study of radionuclide contaminants in surface and subsurface waters, as well as in zooplankton and fish, off Japan in June 2011. A major finding is detection of Fukushima-derived (134)Cs and (137)Cs throughout waters 30-600 km offshore, with the highest activities associated with near-shore eddies and the Kuroshio Current acting as a southern boundary for transport. Fukushima-derived Cs isotopes were also detected in zooplankton and mesopelagic fish, and unique to this study we also find (110 m)Ag in zooplankton. Vertical profiles are used to calculate a total inventory of ~2 PBq (137)Cs in an ocean area of 150,000 km(2). Our results can only be understood in the context of our drifter data and an oceanographic model that shows rapid advection of contaminants further out in the Pacific. Importantly, our data are consistent with higher estimates of the magnitude of Fukushima fallout and direct releases [Stohl et al. (2011) Atmos Chem Phys Discuss 11:28319-28394; Bailly du Bois et al. (2011) J Environ Radioact, 10.1016/j.jenvrad.2011.11.015]. We address risks to public health and marine biota by showing that though Cs isotopes are elevated 10-1,000× over prior levels in waters off Japan, radiation risks due to these radionuclides are below those generally considered harmful to marine animals and human consumers, and even below those from naturally occurring radionuclides.

Application of cross-flow ultrafiltration for the determination of colloidal abundances in suboxic ferrous-rich ground waters.

A suboxic groundwater from a sandy coastal aquifer was sampled using a new air free, large volume sampling method. Subsequent processing for size fractionation was completed with a modified cross-flow ultrafiltration (CFF) system equipped with a 1 kDa CFF membrane. By purging the CFF system with nitrogen, no oxygen was able to reach the sample. With this optimization, the sample was processed with higher than 90% recovery in terms of both iron and phosphate. Only about 4% of iron and 20% of phosphate in the filtered (0.2 microm) groundwater sample was found to be in colloidal form in the groundwater. In contrast, if no care was taken to maintain the suboxic environment of the original sample, iron was rapidly and completely oxidized and subsequently adsorbed to the CFF membrane. Other elements, such as phosphorus, were also lost to the CFF membrane to a substantial degree, and the mechanism is most likely coprecipitation with iron oxides. This study thus strongly supports the importance of maintaining ambient redox conditions during sampling and fractionation, especially for the determinations of colloid abundances in groundwater.

Plutonium in groundwater at the 100K-Area of the U.S. DOE Hanford Site.

We examined the concentration, size distribution, redox state and isotopic composition of plutonium (Pu) in groundwater at the 100K-Area at the U.S. Department of Energy's (DOE) Hanford Site. Total concentrations of Pu isotopes were extremely low (10(-4) to 10(-6) pCi/kg, approximately 10(4) to 10(6) atoms/kg) but measurable for the first time in the 100K-Area wells using mass spectrometric analyses that are much more sensitive than alpha spectroscopy methods used previously. Size fractionation data from two wells suggest that 7-29% of the Pu is associated with colloids, operationally defined here as particles between 1 kDa-0.2 microm in size. These colloids were collected using a 1 kDa cross-flow ultrafiltration (CFF) system developed specifically for groundwater actinide studies to include careful controls both in the field and during processing to ensure in situ geochemical conditions are maintained and size separations can be well characterized. Pu in this colloidal fraction was exclusively in the more reduced Pu(III/IV) form, consistent with the higher affinity of Pu in the lower oxidation states for particle surfaces. While the overall concentrations of Pu were low, the Pu isotopic composition suggests at least two local sources of groundwater Pu, namely, local Hanford reactor operations at the 100K-Area and spent nuclear fuel from the N-reactor, which was stored in concrete pools at this site. Differences between this site and the Savannah River Site (SRS) are noted, since groundwater Pu at the F-Area seepage basin at SRS has been found using these same methods, to be characterized by lower colloidal abundances and higher oxidation states. This difference is not directly attributable to groundwater redox potential or geochemical conditions, but rather the physical-chemical difference in Pu sources, which at SRS appear to be dominated downstream from the seepage basins by decay of 244Cm, resulting in more oxidized forms of 240Pu. There is no clear evidence for colloid facilitated transport of Pu in groundwater at the Hanford Site, since downstream wells have both an order of magnitude lower concentrations of Pu and a lower fractional colloidal distribution.

The effects of iron fertilization on carbon sequestration in the Southern Ocean.

An unresolved issue in ocean and climate sciences is whether changes to the surface ocean input of the micronutrient iron can alter the flux of carbon to the deep ocean. During the Southern Ocean Iron Experiment, we measured an increase in the flux of particulate carbon from the surface mixed layer, as well as changes in particle cycling below the iron-fertilized patch. The flux of carbon was similar in magnitude to that of natural blooms in the Southern Ocean and thus small relative to global carbon budgets and proposed geoengineering plans to sequester atmospheric carbon dioxide in the deep sea.