Kazuya Tanaka

Size distribution studies of 137Cs in river water in the Abukuma Riverine system following the Fukushima Dai-ichi Nuclear Power Plant accident

The occurrence of (137)Cs in size fractionated samples in river water from the Abukuma River system, (the Kuchibuto and Abukuma Rivers, five sampling events for three sites) was studied from June 2011--approximately some three months after the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident until December 2012. The total concentration of (137)Cs (mBq/L) in river water was generally high at the upper stream site in the Yamakiya District within the evacuation/off-limits zone. The (137)Cs concentration was about 1Bq/L for the first sampling campaign (June 2011) at all sites, but then decreased substantially to about one-tenth of that by the time of a second sampling campaign (November or December 2011). The (137)Cs in the <0.45 μm fraction was present exclusively as a dissolved species rather than as a species adsorbed on suspended solids or complexed with organic materials. The contribution of the dissolved fraction ranged from 1.2 to 48.9% (averaged 20%) of the total concentration of (137)Cs throughout the observation period. The maximum contribution of (137)Cs was found in the silt size fraction (3-63 μm), which can be explained by the relatively large Kd values and the suspended solids (SS) concentration of this size fraction. Although the concentration (Bq/g) of (137)Cs in each size fraction did not show any significant trends and/or variations for any of the sampling campaign, Kd values for each site increased with time. Furthermore, it was found that the Kd values decreased with distance from the headstream in the off-limits zone. Thus, the data acquired in this study give an overview of the radiological situation for Fukushima including temporal and spatial variation of radiocaesium in a natural riverine system, within a few years after the accident.

Heterogeneous distribution of radiocesium in aerosols, soil and particulate matters emitted by the Fukushima Daiichi Nuclear Power Plant accident: retention of micro-scale heterogeneity during the migration of radiocesium from the air into ground and river systems

We analyzed 137Cs in aerosols, rock, soil and river suspended sediment collected after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. Based on the results, we discuss the post-event behavior and transportation of radiocesium in the environment from the air into ground and river systems. First, radionuclides were emitted from the FDNPP as airborne ‘hot’ particles, which contained water-soluble fractions of radiocesium. Radiocesium was still present in a water-soluble fraction after deposition on the ground. Subsequent interaction of the ‘hot’ particles with water (e.g. rainfall) dissolved and strongly fixed the radiocesium on rock and soil particles, thus changing the radiocesium into insoluble forms. The distribution of ‘hot spots’ was possibly controlled by the initial position of deposition on the ground. Consequently, ‘hot spots’ were studded on the rock surface rather than being uniformly distributed. The distribution of radiocesium in river suspended particles was not homogeneous during water transportation, reflecting the heterogeneity of radiocesium in rock and soil. Leaching experiments demonstrated that radiocesium in rock, soil and river suspended sediment was fairly insoluble, showing that the adsorption reaction is irreversible. The micro-scale heterogeneous distribution of radiocesium in aerosols, soil and suspended particles was due to the presence of ‘hot’ particles in aerosols. Dissolution of radiocesium in the ‘hot’ particles in the aerosols and subsequent irreversible adsorption onto the soil particle complex are responsible for the preservation of the heterogeneity both in soil and in river suspended particles.

Local distribution of radioactivity in tree leaves contaminated by fallout of the radionuclides emitted from the Fukushima Daiichi Nuclear Power Plant

We analyzed fresh and dead leaves collected in forests in Fukushima after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, using autoradiography. Both fresh and dead leaves of Cryptomeria japonica were contaminated by radionuclides (134Cs and 137Cs). Contamination of the fresh leaves was possibly attributed to interception of radionuclides by tree canopies, whereas the dead leaves indicated the direct deposition of radionuclides by fallout and/or washout of radionuclides intercepted by tree canopies. Translocation of radiocesium from a contaminated branch to new leaves growing after the FDNPP accident was not clearly observed, although transfer of radiocesium from leaf parts to male flowers occurred. Fallen leaves of Quercus serrata, which started growing after the FDNPP accident, did not show radioactivity, indicating that significant amounts of translocation from other parts to new leaves did not occur. Fallen leaves of Q. serrata collected from a litter showed hot spots originating from direct fallout. Needles of Pinus densiflora were also contaminated by fallout. Leaching with pure water removed soluble fractions of radiocesium and hot particles from the surface of the contaminated leaves, but significant amounts of radioactivity remained. This means that foliar absorption occurred in both fresh and dead leaves. Further leaching experiments using surfactant and acetone could not remove the remaining radiocesium from the leaves. The leaching experiments indicate that radiocesium in the contaminated leaves is strongly fixed in leaf tissues and is not readily released unless leaf tissues are decomposed.

Investigation of Spatial Distribution of Radiocesium in a Paddy Field as a Potential Sink

Surface soils, under various land uses, were contaminated by radionuclides that were released by the Fukushima Daiichi Nuclear Power Plant accident. Because paddy fields are one of the main land uses in Japan, we investigated the spatial distribution of radiocesium and the influence of irrigation water in a paddy field during cultivation. Soil core samples collected at a paddy field in Fukushima showed that plowing had disturbed the original depth distribution of radiocesium. The horizontal distribution of radiocesium did not show any evidence for significant influence of radiocesium from irrigation water, and its accumulation within the paddy field, since the original amount of radiocesium was much larger than was added into the paddy field by irrigation water. However, it is possible that rainfall significantly increases the loading of radiocesium.

Zinc Sorption During Bio-oxidation and Precipitation of Manganese Modifies the Layer Stacking of Biogenic Birnessite

The formation and structural evolution of fungal mediate biogenic birnessite are dynamic processes. Although the associations of Zn with the pre-formed biogenic Mn oxides are relatively well understood, the reactivity of the intermediate precipitate at the initial stage of Mn bio-oxidation appears to differ from the final precipitate. In the present work, Zn sorption during precipitation of biogenic Mn oxides was investigated contrasting Zn sorption to pre-formed biogenic Mn oxides, using the Mn-oxidizing fungus Paraconiothyrium sp. WL-2. A substantially higher Zn uptake was found during precipitation of biogenic Mn oxides compared to Zn sorption to pre-formed biogenic Mn oxides. The presence of Zn during Mn oxidation resulted in a biogenic Mn oxide with reduced ordering in the c-axis. The precipitate was identified by X-ray diffraction (XRD) as a layer-type Mn oxide with structural properties similar to hexagonal birnessite. Extended X-ray absorption fine structure (EXAFS) spectroscopy showed that Zn forms triple-corner-sharing tetrahedral coordination (IVTCS-Zn) complexes on the surface of birnessite, which may inhibited layer stacking of birnessite in the final products. This study emphasizes the importance of the intermediate precipitates on Zn sorption, and provides insight regarding the dynamic interaction between Zn and Mn oxide in the process of microbiological oxidation. Supplemental materials are available for this article. Go to the publishers online edition of Geomicrobiology Journal to view the supplemental file.

Trophic Position and Metabolic Rate Predict the Long-Term Decay Process of Radioactive Cesium in Fish: A Meta-Analysis

Understanding the long-term behavior of radionuclides in organisms is important for estimating possible associated risks to human beings and ecosystems. As radioactive cesium (137Cs) can be accumulated in organisms and has a long physical half-life, it is very important to understand its long-term decay in organisms; however, the underlying mechanisms determining the decay process are little known. We performed a meta-analysis to collect published data on the long-term 137Cs decay process in fish species to estimate biological (metabolic rate) and ecological (trophic position, habitat, and diet type) influences on this process. From the linear mixed models, we found that 1) trophic position could predict the day of maximum 137Cs activity concentration in fish; and 2) the metabolic rate of the fish species and environmental water temperature could predict ecological half-lives and decay rates for fish species. These findings revealed that ecological and biological traits are important to predict the long-term decay process of 137Cs activity concentration in fish.

Recovery and Separation of Rare Earth Elements Using Salmon Milt

Recycling rare earth elements (REEs) used in advanced materials such as Nd magnets is important for the efficient use of REE resources when the supply of several REEs is limited. In this work, the feasibility of using salmon milt for REE recovery and separation was examined, along with the identification of the binding site of REEs in salmon milt. Results showed that (i) salmon milt has a sufficiently high affinity to adsorb REEs and (ii) the adsorption capacity of the milt is 1.04 mEq/g, which is comparable with that of commercial cation exchange resin. Heavier REEs have higher affinity for milt. A comparison of stability constants and adsorption patterns of REEs discussed in the literature suggests that the phosphate is responsible for the adsorption of REE in milt. The results were supported by dysprosium (Dy) and lutetium (Lu) LIII-edge extended x-ray absorption fine structure (EXAFS) spectroscopy. The REE-P shell was identified for the second neighboring atom, which shows the importance of the phosphate site as REE binding sites. The comparison of REE adsorption pattern and EXAFS results between the milt system and other adsorbent systems (cellulose phosphate, Ln-resin, bacteria, and DNA-filter hybrid) revealed that the coordination number of phosphate is correlated with the slope of the REE pattern. The separation column loaded with milt was tested to separate REE for the practical use of salmon milt for the recovery and separation of REE. However, water did not flow through the column possibly because of the hydrophobicity of the milt. Thus, sequential adsorption–desorption approach using a batch-type method was applied for the separation of REE. As an example of the practical applications of REE separation, Nd and Fe(III) were successfully separated from a synthetic solution of Nd magnet waste by a batch-type method using salmon milt.

Immobilization of selenium by biofilm of Shewanella putrefaciens with and without Fe(III)-citrate complex

To investigate the effect of biofilms on selenium migration, we examined selenite reduction by biofilms of an iron-reducing bacterium, Shewanella putrefaciens, under anaerobic conditions. The biofilms were grown under static conditions on culture cover glasses coated with poly-L-lysine. Optical microscopic observation of the biofilms after staining with 0.1% crystal violet solution revealed that the cells were surrounded by filamentous extracellular polymer substances. Exposure of the biofilms to aqueous selenite resulted in the formation of red precipitates, which were assigned to nanoparticulate elemental selenium using X-ray absorption near-edge structure analysis. Micrographic observation showed that the precipitates immobilized at the biofilms. We also examined the selenite reduction in the presence of Fe(III)-citrate complex. In this case, a dark brown precipitate formed at the biofilms. X-ray absorption near-edge structure analysis revealed that the precipitate was a mixed compound with elemental selenium and iron selenide. These findings indicate that biofilms of iron-reducing bacteria in the environment can immobilize selenium by reducing Se(IV) to Se(0), and Fe(III)-citrate complex promotes the reduction of Se(0) to Se(-II).

Cobalt(II) Oxidation by Biogenic Mn Oxide Produced by Pseudomonas sp. Strain NGY-1

Oxidation of Co by Mn oxide has been investigated using abiotically synthesized Mn oxide. However, oxidation of Co by biogenic Mn oxide is not well known. In this study, we isolated a Mn-oxidizing bacterium (Pseudomonas sp.), designated as strain NGY-1, from stream water. Sorption experiments on Co were carried out using biogenic Mn oxide produced by strain NGY-1. Similar sorption experiments were also conducted using a synthetic analogue of δ-MnO2. Sorption of Co on δ-MnO2 was faster and stronger than that on biogenic Mn oxide, which was possibly due to their structural difference and/or the presence of bacterial cells in biogenic Mn oxide. X-ray absorption near-edge structure spectra clearly demonstrated that Co was oxidized from the divalent to the trivalent state on biogenic Mn and δ-MnO2. The oxidation property of both the biogenic Mn oxide and δ-MnO2 was stronger under circumneutral conditions than under acidic conditions. Linear combination fitting using divalent and trivalent Co reference materials suggested that ∼90% of Co was oxidized at pH ∼ 6, whereas ∼80% was oxidized at pH ∼ 3. Oxidation properties of the biogenic Mn oxide and δ-MnO2 were similar, but Co(II) oxidation by biogenic Mn oxide was slower than that by δ-MnO2. The difference of Co oxidation may be caused by the coexisting bacterial cells or structural differences in the Mn oxides. Supplemental materials are available for this article. Go to the publishers online edition of Geomicrobiology Journal to view the supplemental file.

Adsorption of ytterbium onto Saccharomyces cerevisiae fungal cells: A pH-dependent contribution of phosphoryl functional group

The adsorption of ytterbium on the cells of yeast Saccharomyces cerevisiae has been studied by batch type experiment by changing solution pH. The Yb adsorption species on the yeast cell wall of the S. cerevisiae was determined by extended X-ray absorption fine structure spectroscopy combined with a linear combination analysis at various pHs. The results indicated that the contribution of Yb-phosphoryl species was constant between pH 3 and 5, strongly suggesting that most of the Yb was associated with undeprotonated phosphoryl functional groups.