Estimation of accumulation potential for tritium in olive flounder on exposure of treated water derived from Fukushima Daiichi Nuclear Power Station: Tritium transfer from seawater and food chain into organically bound tritium in the targeted fish.

This study estimated the accumulation potential of tritium, a major radionuclide released from the Fukushima Daiichi Nuclear Power Station (FDNPS), into the olive flounder as organically bound tritium (OBT) using a computer simulation model. In this estimation, two transfer pathways into the OBT were assumed: formation from tritiated water (HTO) in the tricarboxylic acid (TCA) cycle, and ingestion of OBT through the food chain (from phytoplankton, small fish, to the flounder). The food chain structure was reconstructed based on fish growth model. The OBT concentration in the flounder was estimated on three scenarios: Tritium was supplied to the flounder as only HTO in seawater (Scenario 1), as HTO in seawater and OBT formed from HTO in the small fish (Scenario 2), and as HTO in seawater and OBT accumulated in the small fish through the formation and ingestion of OBT in phytoplankton (Scenario 3). The estimated OBT concentrations in the flounder were in the following order: Scenario 3 > 2 > 1. The ratio of the estimated concentration in Scenario 1 to that in Scenario 3 reached a certain value (66 % after a year from the start of HTO exposure), indicating that the tritium transfer from the seawater into the flounder more significantly contributed to this concentration than ingestions of the small fish and the phytoplankton. Additionally, the difference between the estimations of Scenarios 1 and 2 is significantly larger than that between Scenarios 2 and 3. This suggests that phytoplankton contributed weakly to the OBT concentration in the flounder compared to the small fish.

Sequential loss-on-ignition as a simple method for evaluating the stability of soil organic matter under actual environmental conditions.

Soil organic matter (SOM) is one of the largest carbon (C) reservoirs on Earth, and therefore its stability attracts a great deal of interest from the perspective of the global C cycle. This study examined the applicability of loss-on-ignition with a stepwise increase in temperature (SIT-LOI) of soil to evaluate the stability of SOM using soil samples having different organic matter (OM) and mineral contents and different mean residence times (MRTs) for SOM. The responses of SOM to the SIT-LOI varied depending on the samples but were all successfully approximated by a liner regression model as a function of the temperature of LOI. The slope value in the liner model that determines the residual potential of carbon during the SIT-LOI highly correlated with MRT of SOM, suggesting that this value reflects the overall stability of SOM over a range of soil properties. This hypothesis was consistent with the observation that Δ14C values of SOM decreased with increasing LOI temperature and thus, older, slower-cycling SOM was preferentially left in the soil samples by SIT-LOI. Additionally, the hypothesis was also supported by the significant correlations (p < 0.01) between the slope value and OM and mineral contents in the samples because these components are considered to regulate SOM stability. In addition to the regression analysis of the SIT-LOI data, changes in carbon to nitrogen (C/N) and carbon to hydrogen (C/H) ratios and stable carbon isotope signatures (δ13C) of the samples were investigated. The results suggest that the mineral association of SOM is an important factor characterizing the response of SOM to LOI. Hence, it was concluded that SIT-LOI is a simple and useful method for evaluating the stability of SOM under actual environmental conditions.

Investigation of changes in the iodine concentrations of oceanic sediment and terrestrial soil samples after thermal drying.

To certify the suitability of pretreatment by thermal drying to measure iodine concentrations of oceanic sediment and terrestrial soil samples, changes in iodine concentrations after drying (50, 80 or 85, and 110 °C for 48 h) were examined using the samples in addition to a terrestrial plant (pine needles), which was selected as an intact organic sample. The iodine concentrations per wet weight of the sediment and soil samples processed by thermal drying were comparable to those of the raw samples at all temperatures. However, the concentrations of the plant samples dried at 85 and 110 °C were lower than those of the raw samples. The lower concentrations of the plant samples at higher temperatures were considered to be derived from the volatilization of a part of the plant's organic matter. Finally, these results suggested that the iodine concentrations in oceanic sediment and terrestrial soil samples scarcely change after thermal drying at 110 °C, although the concentrations may decrease when these samples include high contributions of fresh organic matter.

Concentrations of iodine-129 in livestock, agricultural, and fishery products around spent nuclear fuel reprocessing plant in Rokkasho, Japan, during and after its test operation.

Concentrations of iodine-129 (129I) and atomic ratios of 129I/127I in livestock (grass and milk), agricultural (cabbage, Japanese radish, and rice), and fishery (flatfish and brown alga) products collected from locations around the first Japanese commercial spent nuclear fuel reprocessing plant in Rokkasho were measured from 2006 to 2016. The actual spent nuclear fuel rods were cut and processed to test the functioning of the plant that discharged controlled amounts of 129I to the atmosphere and coastal seawater during the period from 2006 to 2008 (the "cutting period"). Statistically significant increases in 129I concentration and 129I/127I ratio were observed during the cutting period in livestock products and flatfish. On the other hand, these parameters were statistically comparable during and after the cutting period in the other products. The radiation dose through the ingestion of the maximum 129I concentrations, measured in the different products, was estimated to be in the nanoSievert per year level. This value is much smaller than 1 mSv yr-1, which is the permissible authentic radiation dose for the general public. The 129I levels in the samples, especially in milk and flatfish, are discussed in context of the 129I discharge history from the plant.

Vertical and lateral transport of particulate radiocesium off Fukushima.

Transport processes of particulate radiocesium were investigated using a sediment trap deployed at about 100 km east of the Fukushima Daiichi Nuclear Power Plant. A sediment trap was installed at 873 m depth of the station (119 m above the bottom), and time-series sampling of sinking particles was carried out from August, 2011 to June, 2013. The accident-derived radiocesium was detected from sinking particles over two years after the accident. Observed 137Cs flux was highest in September 2011 (98 mBq m(-2) day(-1): decay-corrected to March 11, 2011), and decreased over time with seasonal fluctuations. Particulate fluxes of radiocesium were mainly affected by two principal processes. One was the rapid sinking of radiocesium-bound particles (moderate mode). This mode was dominant especially in the early postaccident stage, and was presumed to establish the distribution of radiocesium in the offshore seabed. Another mode was observed in winter, and secondary transport of particles attributed to turbulence near the seabed increased fluxes of particulate radiocesium (turbulence mode). Although the latter process would not drastically change the distribution of sedimentary radiocesium in the short term, attention should be paid as this key process redistributing the accident-derived radiocesium may cumulatively affect the long-term distribution.

Comparison of dissolved iodine measurements in seawater between inductively coupled plasma mass spectrometry and voltammetry.

Two analytical methods, inductively coupled plasma mass spectrometry (ICP-MS) combined with high-performance liquid chromatography (HPLC) and voltammetry (VM), for three chemical species of dissolved iodine (iodide, iodate, and total dissolved iodine: TDI) were compared for dozens of coastal seawater samples owing to the compatibility of data between both methods. The median differences in the measured concentrations of TDI, total inorganic dissolved iodine (TII, the sum of iodide and iodate), and iodate between ICP-MS and VM were equivalent to 9.2, 13, and 14%, respectively. These differences were within the ranges that could be explained by the repeated-measurement precision of each measurement method for TDI, TII, and iodate. The difference for iodide was 19%, which was larger than the value based on the repeated-measurement precision for both methods. This is considered to be caused by the chemical instability and lower concentrations of iodide compared to other iodine species in seawater, in addition to the heterogeneity of natural samples. Finally, both methods provided reasonable measurement values for the iodine concentration in natural seawater samples.

Evaluating production rates of particulate organic hydrogen by marine phytoplankton for estimating phytoplanktonic productivity of organically bound tritium.

To estimate the production potential of organically bound tritium (OBT) by phytoplankton from tritiated water in coastal areas adjacent to the Fukushima Daiichi Nuclear Power Plant (FDNPP), phytoplanktonic production rates of particulate organic hydrogen (POH) were evaluated in laboratory and field experiments using stable isotope tracers (2H and 13C). In the laboratory experiment, the production rate of POH was evaluated for five types of phytoplankton cultivated cultures (two diatoms, Haptophyceae, Chlorophyceae, and Cryptophyceae) at two temperatures (15 °C and 25 °C) and two 2H concentrations in the medium (1 and 5%). Additionally, the production rate of POH was especially focused on non-exchangeable POH (NE-POH) which is the chemical form of hydrogen connected tightly to organic matter. The production rates of NE-POH in the laboratory experiment varied (0.10 to 36 µmol L-1 d-1 µg-Chl a-1) with the productivity of particulate organic carbon, phytoplankton species, and temperature, with negligible influence of 2H concentrations. In the field experiment, in situ incubation of coastal seawater at water depths of 1 and 20 m with isotope tracers under light and dark conditions, respectively, was performed thrice (November 2021, May 2022, and October 2022) on the Pacific coastal ocean approximately 2 km from the land of northeast Japan. We observed variation in the production rate of POH (0.21 to 3.1 µmol L-1 d-1 µg-Chl a-1), which was theoretically explained by the data in the laboratory experiment. Using the phytoplanktonic production rate of POH obtained in this study, OBT production by phytoplankton and the subsequent accumulation potential of OBT in sediments in the coastal area adjacent to FDNPP were tentatively estimated, results of which suggested this potential to be small.

Organic matter composition regulates residual potential of organic carbon of the seagrass Zostera marina L. during its decomposition process in seawater.

Although the seagrass Zostera marina L. (Z. marina) is expected to significantly contribute to environmental carbon dynamics, the residual potential of organic carbon (Corg) in this plant during its decomposition process in seawater remains insufficiently understood. In this study, the factors regulating this potential were examined by evaluating Z. marina decomposition in seawater and conducting a multiple regression analysis on data from the experiment as well as the original plant organic matter composition. The residual ratio during the decomposition experiment (RDEC) of carbon in Z. marina for 111 days ranged from 0.30 to 0.84 (n = 16), and the variation resulted from differences in the sampling season of this plant. Regression analysis was conducted to explain the RDEC of carbon using the RDEC of nitrogen, concentrations of carbon, nitrogen, HCl-extractable Corg and nitrogen, contributions of carbohydrate (CCAR) of total and non-structural fractions and lipid (CLIP) to carbon concentration. The RDEC of carbon was most adequately fitted using a multiple regression including three parameters, carbon concentration, CLIP, and CCAR of total carbohydrate with a significant determination coefficient. The former two parameters (carbon concentration and CLIP) have negative coefficients, indicating that these parameters correspond to bacterially available Corg in Z. marina in the regression analysis. The latter parameter (CCAR of total carbohydrate) shows a positive coefficient that indicates recalcitrant Corg in the regression. Parameters related to nitrogen were not included in the regression formula, although this element is reportedly an important parameter regulating the environmental decomposition rate of Corg. Finally, we suggested that total carbon, carbohydrate, and lipid are especially important factors to regulate the environmental residual potential of Z. marina Corg among organic components of this plant.

EXPERIMENTAL EVALUATION OF DISTRIBUTION OF 14C PHOTOASSIMILATED INTO CARBOHYDRATES IN DIFFERENT GROWTH STAGES OF FRUIT-BEARING APPLE SHOOTS USING A 13CO2 IN-SITU EXPOSURE SYSTEM.

In this study, we aimed to investigate the photoassimilation process of 14CO2 into agricultural plants through determining the photoassimilated carbohydrate-13C in each part (leaves, current branch and fruit) of the fruit-bearing apple shoots exposed to 13CO2 in different growth stages (early and late fruit development stages). The carbohydrate content was assessed as soluble (ethanol-extracted fraction) and other (HCl-extracted and residual fractions) components. The total (i.e. sum of the three fractions) bulk carbohydrate concentrations in all parts of the shoots were statistically similar between different growth stages. The changes in the concentration of 13C-labeled soluble carbohydrate (i.e. ethanol-extracted fraction) to the total content between different growth stages were statistically unclear among all parts of the shoot. These results suggest that the distribution ratio of photoassimilated 13C in soluble and other components in the apple shoot was thereabout constantly independent of the growth stages.

Investigation of ratio of carbon to hydrogen (C/H ratio) in agricultural plants for further estimation of their productivity of organically bound tritium.

The carbon to hydrogen ratio (C/H ratio, w/w) in plants is a key factor in estimating the amount of hydrogen in the photosynthetic product. The amount of hydrogen calculated from photosynthetic model estimation associated with the C/H ratio is an essential parameter of the estimation model of productivity of organically bound tritium (OBT) by plants. To propose a sophisticated estimation model of OBT by agricultural plants, temporal changes in the C/H ratio of six plant species (Japanese radish, cabbage, orchard grass, paddy field rice, apple, and radish) during their cultivation were investigated for each plant part. The C/H ratio in the plants cultivated in the field and growth chamber generally exceeded 6, which is the value for the primary photosynthetic monosaccharides, such as glucose and fructose (both chemical formulae, C6H12O6). In the vegetative parts (e.g. Japanese radish leaves, cabbage leaves and roots, rice leaves and roots, and radish leaves and fine roots) the C/H ratio fluctuated irregularly or remained constant within an approximate range of 6.6-7.3 during cultivation. The C/H ratio in enlarged organs (e.g. Japanese radish root, rice ear, apple fruit, and radish main root) decreased continuously, approaching 6. These results suggest that the C/H ratio can be generally set as approximately 6.9 except for enlarged organs, in which the ratio may change over time during cultivation, within an approximate range of 6-7.

Flux and pathway of iodine dissolution from brackish lake sediment in the northeast of Japan.

Sediment is one of the most important entities controlling the environmental dynamics of iodine. We previously evaluated the dissolution flux of iodine from aquatic sediment to its overlying water in a brackish lake through an incubation experiment with a sediment core sample, reporting the regulation factors of this flux, such as the temperature and oxygenic conditions. In this study, factors controlling the seasonal variation in the dissolution flux of iodine were investigated via an incubation experiment using the sediment core samples collected in autumn and summer. The dissolution flux in this study was significantly smaller than that reported in our previous study. The iodine concentration detected in the overlying water of the sediment during incubation in this study was positively correlated with the concentrations of some inorganic ions, such as Na+, Cl-, and SiO42-, while these correlations were not confirmed in our previous study. As the dissolution of sedimentary iodine includes two pathways, which are the diffusion of sedimentary pore water and degradation of organic matter on surface sediment, correlations potentially indicate that the dissolution flux estimated in this study has a larger contribution from sedimentary pore water than that in our previous study. In addition, the higher flux estimated in our previous study was considered to be caused by the larger contribution from iodine derived from the degradation of phytoplanktonic organic matter on surface sediment. Assuming that the dissolution fluxes estimated in the previous and present studies are representative of the fluxes during and excluding the high productivity season in Lake Obuchi, respectively, we estimated the annual flux at 2.7 g y-1 m-2, which is comparable with our previous estimation.

Evaluation of radioiodine (129I) dissolution from sediment of a brackish lake beside a spent nuclear fuel reprocessing plant in Japan.

Dissolution fluxes of stable (127I) and radioactive (129I) isotopes of iodine from a brackish lake sediment beside a spent nuclear fuel reprocessing plant in Japan were evaluated through two kinds of experiments: incubation using a sediment core sample for 24 h, and observation of 127I and 129I concentrations in sedimentary pore water. For 127I, the dissolution flux evaluated in the incubation experiment was comparable with that obtained from the vertical gradient of 127I concentration in pore water in the observation experiment. This suggests that degradation of organic matter in the surface sediment is an important source of dissolved 127I found in the water. For 129I, the dissolution flux estimated in the incubation experiment showed negative values, indicating the transfer of 129I to the sediment from the overlying water (i.e., absorption). Moreover, the flux evaluated from the observation experiment was positive. This result suggests that degradation of organic matter in the surface sediment is scarcely important to the supply of 129I from the sediment to the water in the studied lake. The dissolution flux of 129I estimated in the observation experiment was smaller than the absorption flux of 129I in the incubation experiment. This potentially indicates that the dissolution of sedimentary 129I does not significantly change 129I concentrations in the water and sediment of the lake. This hypothesis was consistent with previous research conducted for the studied lake.

Evaluation of dissolution flux of iodine from brackish lake sediments under different temperature and oxygenic conditions.

Dissolution flux of iodine from aquatic sediments in a brackish lake (Lake Obuchi), facing the Pacific Ocean and adjacent to a nuclear fuel reprocessing plant in northeast Japan, was evaluated using incubation experiments on sediment core samples. The experiments were performed under three different temperatures (29, 17, and 6 °C) and oxygenic (air flow, N2 gas flow, and untreated) conditions for 48 h. The total dissolved iodine (TDI) concentration (i.e., the sum of iodide, iodate, and dissolved organic iodine, DOI) increased under all temperatures and oxygenic conditions in the first 6 h of incubation. From 6 to 27 h, noticeable increases in TDI concentration only occurred at high temperatures. Dissolution fluxes of iodine estimated by linear regression analysis of the measured TDI concentration in the first 6 h were always higher than those estimated in the first 27 h. This result indicates that dissolution flux of iodine should be evaluated through short-term (within several hours) incubation experiments because absorption reactions which transport iodine from the overlying water back to the sediment become active in the long-term. No substantial difference in dissolution flux, estimated by TDI concentration, was observed under different oxygenic conditions in the first 6 h. However, dissolution flux increased significantly with an increase in temperature. Increases in flux and temperature were significantly and positively correlated (R2 = 0.90), suggesting that temperature was the dominant factor that regulated iodine flux during the incubation. Changes in TDI concentration at all temperatures and oxygenic conditions corresponded to those in iodide concentration, indicating that iodide was the main form of iodine dissolved from the sediments. In later stages of the experiments, from 27 to 48 h, the TDI concentration in overlying water increased only at high temperature, while concentrations at medium and low temperatures remained constant or decreased. In particular, oxic experiments showed substantial decreases in iodide concentration at medium and low temperatures. This suggests that oxic conditions promote the absorption of iodine from the overlying water to the sediments. Finally, the dissolution flux of radioiodine (iodine-129) from the sediments of Lake Obuchi to the overlying water was estimated by combining these results with data from earlier studies. The results suggest that only 0.006% of the iodine-129 accumulated in the sediments is released through dissolution to the overlying water per year, suggesting that this radioactive isotope is essentially stable in the sediments.

Distribution and fate of 129I in the seabed sediment off Fukushima.

In this study, seabed sediment was collected from 26 stations located within 160 km from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) during the 2 years which followed the FDNPP accident of March 2011 and the concentrations of 129I and 137Cs were measured. By comparing the distribution of these two radionuclides with respect to their different geochemical behaviors in the environment, the transport of accident-derived radionuclides near the seafloor is discussed. The concentration of 129I in seabed sediment recovered from offshore Fukushima in 2011 ranged between 0.02 and 0.45 mBq kg-1, with 129I/137Cs activity ratios of (1.9 ±â€¯0.5) × 10-6 Bq Bq-1. The initial deposition of 129I to the seafloor in the study area was 0.36 ±â€¯0.13 GBq, and the general distribution of sedimentary 129I was established within 6 months after the accident. Although iodine is a biophilic element, the accident-derived 129I negligibly affects the benthic ecosystem. Until October 2013, a slight increase in activity of 129I in the surface sediment along the shelf-edge region (bottom depth: 200-400 m) was observed, despite that such a trend was not observed for 137Cs. The preferential increase of the 129I concentrations in the shelf-edge sediments was presumed to be affected by the re-deposition in the shelf-edge sediments of 129I desorbed from the contaminated coastal sediment. The results obtained from this study indicate that 129I/137Cs in marine particles is a useful indicator for tracking the secondary transport of accident-derived materials, particularly biophilic radionuclides, from the coast to offshore areas.