J. Patrick Laceby

Radiocesium transfer from hillslopes to the Pacific Ocean after the Fukushima Nuclear Power Plant accident: A review

The devastating tsunami triggered by the Great East Japan Earthquake on March 11, 2011 inundated the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) resulting in a loss of cooling and a series of explosions releasing the largest quantity of radioactive material into the atmosphere since the Chernobyl nuclear accident. Although 80% of the radionuclides from this accidental release were transported over the Pacific Ocean, 20% were deposited over Japanese coastal catchments that are subject to frequent typhoons. Among the radioisotopes released during the FDNPP accident, radiocesium ((134)Cs and (137)Cs) is considered the most serious current and future health risk for the local population. The goal of this review is to synthesize research relevant to the transfer of FDNPP derived radiocesium from hillslopes to the Pacific Ocean. After radiocesium fallout deposition on vegetation and soils, the contamination may remain stored in forest canopies, in vegetative litter on the ground, or in the soil. Once radiocesium contacts soil, it is quickly and almost irreversibly bound to fine soil particles. The kinetic energy of raindrops instigates the displacement of soil particles, and their bound radiocesium, which may be mobilized and transported with overland flow. Soil erosion is one of the main processes transferring particle-bound radiocesium from hillslopes through rivers and streams, and ultimately to the Pacific Ocean. Accordingly this review will summarize results regarding the fundamental processes and dynamics that govern radiocesium transfer from hillslopes to the Pacific Ocean published in the literature within the first four years after the FDNPP accident. The majority of radiocesium is reported to be transported in the particulate fraction, attached to fine particles. The contribution of the dissolved fraction to radiocesium migration is only relevant in base flows and is hypothesized to decline over time. Owing to the hydro-meteorological context of the Fukushima region, the most significant transfer of particulate-bound radiocesium occurs during major rainfall and runoff events (e.g. typhoons and spring snowmelt). There may be radiocesium storage within catchments in forests, floodplains and even within hillslopes that may be remobilized and contaminate downstream areas, even areas that did not receive fallout or may have been decontaminated. Overall this review demonstrates that characterizing the different mechanisms and factors driving radiocesium transfer is important. In particular, the review determined that quantifying the remaining catchment radiocesium inventory allows for a relative comparison of radiocesium transfer research from hillslope to catchment scales. Further, owing to the variety of mechanisms and factors, a transdisciplinary approach is required involving geomorphologists, hydrologists, soil and forestry scientists, and mathematical modellers to comprehensively quantify radiocesium transfers and dynamics. Characterizing radiocesium transfers from hillslopes to the Pacific Ocean is necessary for ongoing decontamination and management interventions with the objective of reducing the gamma radiation exposure to the local population.

Novel Insights into Fukushima Nuclear Accident from Isotopic Evidence of Plutonium Spread along Coastal Rivers

The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident led to important releases of radionuclides into the environment, and trace levels of plutonium (Pu) were detected in northeastern Japan. However, measurements of Pu isotopic atom and activity ratios are required to differentiate between the contributions of global nuclear test fallout and FDNPP emissions. In this study, we used a double-focusing sector field ICP-MS to measure Pu atom and activity ratios in recently deposited sediment along rivers draining the most contaminated part of the inland radioactive plume. Results showed that plutonium isotopes (i.e., (239)Pu, (240)Pu, (241)Pu, and (242)Pu) were detected in all samples, although in extremely low concentrations. The (241)Pu/(239)Pu atom ratios measured in sediment deposits (0.0017-0.0884) were significantly higher than the corresponding values attributed to the global fallout (0.00113 ± 0.00008 on average for the Northern Hemisphere between 31°-71° N: Kelley, J. M.; Bond, L. A.; Beasley, T. M. Global distribution of Pu isotopes and (237)Np. Sci. Total. Env. 1999, 237/238, 483-500). The results indicated the presence of Pu from FDNPP, in slight excess compared to the Pu background from global fallout that represented up to ca. 60% of Pu in the analyzed samples. These results demonstrate that this radionuclide has been transported relatively long distances (∼45 km) from FDNPP and been deposited in rivers representing a potential source of Pu to the ocean. In future, the high (241)Pu/(239)Pu atom ratio of the Fukushima accident sourced-Pu should be measured to quantify the supply of continental-originating material from Fukushima Prefecture to the Pacific Ocean.

The impact of typhoons on sediment connectivity: Lessons learnt from contaminated coastal catchments of the Fukushima Prefecture (Japan)

ABSTRACT: Sediment connectivity characterizes the physical transfer of sediment through different geomorphic compartments in catchments due to sediment detachment, transport and deposition. Quantifying and modelling sediment connectivity is therefore a key prerequisite to improving our understanding of the dispersion of particle‐borne contaminants, especially in catchments exposed to highly erosive climates. The objective of this study is to provide novel insights into typhoon impacts on sediment connectivity from hillslopes to rivers. The dispersion of particle‐bound caesium‐137 (137Cs) was investigated in two coastal catchments draining the main contamination plume from the Fukushima Daiichi Nuclear Power Plant accident. Five sampling campaigns were carried out from November 2011 to November 2015, after each typhoon season. The spatial and temporal evolution of 137Cs contamination was investigated through the calculation of 137Cs enrichment ratios in sediment relative to nearby soils. Rainfall erosivity (EI30) associated with the main typhoons that occurred prior to each sampling campaign were computed, mapped, and finally used to improve a topographic‐based index of connectivity. From 2011 to 2015, mean contamination levels in Mano and Niida catchments decreased from 11.9 kBq kg−1 to 3.3 kBq kg−1 and from 34.1 kBq kg−1 to 8.0 kBq kg−1, respectively. Regional mean EI30 ranged from 262 MJ mm ha−1 h−1 for typhoon Jelawat (in 2012) to 1695 MJ mm ha−1 h−1 for typhoon Roke (in 2011). Typhoons Roke (2011) and Etau (2015) showed the highest connectivity from contaminated sources to the rivers, and induced a significant export of sediment to the ocean. In 2013 a slight increase in 137Cs levels in river sediments occurred, likely resulting from initial decontamination works and the occurrence of two consecutive typhoons. Importantly, this research provides new insights into the connectivity of the main sources of sediments contaminated with radiocaesium in Fukushima Prefecture and their temporal evolution, which will help with ongoing decontamination efforts. Copyright

Quantifying sediment sources in a lowland agricultural catchment pond using (137)Cs activities and radiogenic (87)Sr/(86)Sr ratios.

Soil erosion often supplies high sediment loads to rivers, degrading water quality and contributing to the siltation of reservoirs and lowland river channels. These impacts are exacerbated in agricultural catchments where modifications in land management and agricultural practices were shown to accelerate sediment supply. In this study, sediment sources were identified with a novel tracing approach combining cesium ((137)Cs) and strontium isotopes ((87)Sr/(86)Sr) in the Louroux pond, at the outlet of a lowland cultivated catchment (24km(2), Loire River basin, France) representative of drained agricultural areas of Northwestern Europe. Surface soil (n=36) and subsurface channel bank (n=17) samples were collected to characterize potential sources. Deposited sediment (n=41) was sampled across the entire surface of the pond to examine spatial variation in sediment deposits. In addition, a 1.10m sediment core was sampled in the middle of the pond to reconstruct source variations throughout time. (137)Cs was used to discriminate between surface and subsurface sources, whereas (87)Sr/(86)Sr ratios discriminated between lithological sources. A distribution modeling approach quantified the relative contribution of these sources to the sampled sediment. Results indicate that surface sources contributed to the majority of pond (μ 82%, σ 1%) and core (μ 88%, σ 2%) sediment with elevated subsurface contributions modeled near specific sites close to the banks of the Louroux pond. Contributions of the lithological sources were well mixed in surface sediment across the pond (i.e., carbonate sediment contribution, μ 48%, σ 1% and non-carbonate sediment contribution, μ 52%, σ 3%) although there were significant variations of these source contributions modeled for the sediment core between 1955 and 2013. These fluctuations reflect both the progressive implementation of land consolidation schemes in the catchment and the eutrophication of the pond. This original sediment fingerprinting study demonstrates the potential of combining radionuclide and strontium isotopic geochemistry measurements to quantify sediment sources in cultivated catchments.

Investigating the temporal dynamics of suspended sediment during flood events with 7 Be and 210 Pb xs measurements in a drained lowland catchment

Soil erosion is recognized as one of the main processes of land degradation in agricultural areas. High suspended sediment loads, often generated from eroding agricultural landscapes, are known to degrade downstream environments. Accordingly, there is a need to understand soil erosion dynamics during flood events. Suspended sediment was therefore sampled in the river network and at tile drain outlets during five flood events in a lowland drained catchment in France. Source and sediment fallout radionuclide concentrations (7Be, 210Pbxs) were measured to quantify both the fraction of recently eroded particles transported during flood events and their residence time. Results indicate that the mean fraction of recently eroded sediment, estimated for the entire Louroux catchment, increased from 45 ± 20% to 80 ± 20% between December 2013 and February 2014, and from 65 ± 20% to 80 ± 20% in January 2016. These results demonstrate an initial flush of sediment previously accumulated in the river channel before the increasing supply of sediment recently eroded from the hillslopes during subsequent events. This research highlights the utility of coupling continuous river monitoring and fallout radionuclide measurements to increase our understanding of sediment dynamics and improve the management of soil and water resources in agricultural catchments.

Quantifying the dilution of the radiocesium contamination in Fukushima coastal river sediment (2011–2015)

Fallout from the Fukushima Dai-ichi nuclear power plant accident resulted in a 3000-km2 radioactive contamination plume. Here, we model the progressive dilution of the radiocesium contamination in 327 sediment samples from two neighboring catchments with different timing of soil decontamination. Overall, we demonstrate that there has been a ~90% decrease of the contribution of upstream contaminated soils to sediment transiting the coastal plains between 2012 (median – M – contribution of 73%, mean absolute deviation – MAD – of 27%) and 2015 (M 9%, MAD 6%). The occurrence of typhoons and the progress of decontamination in different tributaries of the Niida River resulted in temporary increases in local contamination. However, the much lower contribution of upstream contaminated soils to coastal plain sediment in November 2015 demonstrates that the source of the easily erodible, contaminated material has potentially been removed by decontamination, diluted by subsoils, or eroded and transported to the Pacific Ocean.

Source dynamics of radiocesium-contaminated particulate matter deposited in an agricultural water reservoir after the Fukushima nuclear accident

The Fukushima nuclear accident in Japan resulted in the deposition of radiocesium over forested and rural landscapes northwest of the power plant. Although there have been several investigations into the dynamics of contaminated river sediment, less attention has been paid to the sources of deposited particulate matter in dams and reservoirs. In the Fukushima Prefecture, there are 10 significant dams and over a 1000 reservoirs for both agricultural and surface water management. These reservoirs may have trapped a significant volume of radiocesium-contaminated sediment. Therefore, characterizing the sources of contaminated particulate matter is important for the ongoing management of contamination in the region. Accordingly, the composition of particulate matter deposited in the Mano Dam reservoir, approximately 40km northwest of the power plant, was investigated with the analyses and modelling of carbon and nitrogen stable isotope ratios (δ13C and δ15N), total organic carbon (TOC) and total nitrogen (TN) concentrations. Four sediment cores, with lengths ranging 29-41cm, were sampled in the Mano Dam. Source samples from 46 forest soils, 28 cultivated soils and 25 subsoils were used to determine the source contributions of particulate matter. Carbon and nitrogen parameters were analyzed on all samples and a concentration-dependent distribution modelling approach was used to apportion source contributions. Three of the four cores sampled in the Mano Dam reservoir had distinct radiocesium peaks representative of the initial post-accident wash-off phase. Cultivated sources were responsible for 48±7% of the deposited fine particulate matter whereas forests were modelled to contribute 27±6% and subsoil sources 25±4%. Ongoing decontamination of cultivated sources in the Fukushima region should result in a decrease of contaminated matter deposition in reservoirs.

Plutonium isotopic signatures in soils and their variation (2011-2014) in sediment transiting a coastal river in the Fukushima Prefecture, Japan

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident resulted in a significant release of radionuclides that were deposited on soils in Northeastern Japan. Plutonium was detected at trace levels in soils and sediments collected around the FDNPP. However, little is known regarding the spatial-temporal variation of plutonium in sediment transiting rivers in the region. In this study, plutonium isotopic compositions were first measured in soils (n = 5) in order to investigate the initial plutonium deposition. Then, plutonium isotopic compositions were measured on flood sediment deposits (n = 12) collected after major typhoon events in 2011, 2013 and 2014. After a thorough radiochemical purification, isotopic ratios (240Pu/239Pu, 241Pu/239Pu and 242Pu/239Pu) were measured with a Multi-Collector Inductively Coupled Mass Spectrometer (MC ICP-MS), providing discrimination between plutonium derived from global fallout, from atmospheric nuclear weapon tests, and plutonium derived from the FDNPP accident. Results demonstrate that soils with the most Fukushima-derived plutonium were in the main radiocaesium plume and that there was a variable mixture of plutonium sources in the flood sediment samples. Plutonium concentrations and isotopic ratios generally decreased between 2011 and 2014, reflecting the progressive erosion and transport of contaminated sediment in this coastal river during flood events. Exceptions to this general trend were attributed to the occurrence of decontamination works or the remobilisation of contaminated material during typhoons. The different plutonium concentrations and isotopic ratios obtained on three aliquots of a single sample suggest that the Fukushima-derived plutonium was likely borne by discrete plutonium-containing particles. In the future, these particles should be isolated and further characterized in order to better understand the fate of this long-lived radionuclide in the environment.

Investigating the metal contamination of sediment transported by the 2016 Seine River flood (Paris, France)

Fine sediment transport in rivers is exacerbated during flood events. These particles may convey various contaminants (i.e. metals, pathogens, industrial chemicals, etc.), and significantly impact water quality. The exceptional June 2016 flood of the Seine River (catchment area: 65 000 km2, France), potentially mobilized and deposited contaminated materials throughout the Paris region. Flood sediment deposits (n = 29) were collected along the Seine River and its main tributaries upstream (Yonne, Loing and Marne Rivers) and downstream of Paris (Oise and Eure Rivers). Fallout radionuclides (137Cs, 7Be) were measured to characterize the sources of the material transiting the river, while trace elements (e.g. Cr, Ni, Zn, Cu, As, Cd, Sb, Pb, Tl, Ag) and stable lead isotopes (206Pb/207Pb) were analyzed to quantify the contamination of sediment transported during the flood. In upper sections of the Seine River, sediment mainly originated from the remobilization of particles with a well-balanced contribution of surface and subsurface sources. In the upstream tributaries, sediment almost exclusively originated from the remobilization of subsurface particles. In Paris and downstream of Paris, recently eroded particles and surface sources dominated, suggesting particles were mainly supplied by urban runoff and the erosion of agricultural soils. The highest metal concentrations and Enrichment Factors (EF) were found in the sediment collected in the Loing, Orge and Yvette upstream tributaries. Although these inputs were diluted in the Seine River, an increase in elemental concentrations was observed, progressing downstream through Paris. However, EFs in sediment collected along the Seine River were lower or in the same range of values sampled over the last several decades, reflecting the progressive decontamination of the urbanized Seine River basin.