Distribution of inorganic compositions of Japanese tap water: a nationwide survey in 2019-2024.

A nationwide survey of inorganic components of tap water all over Japan was conducted from 2019 to 2024. In this survey, 1564 tap water samples were collected, and an additional 194 tap water samples were collected from 33 other countries. The water samples were analyzed for 27 dissolved inorganic components, with a primary focus on the distribution of major and trace components, including Ca, Mg, K, Na, Cl-, NO3-, SO42-, total-hardness, Al, Fe, Cu, Mn, and Zn. The Japanese tap water hardness was 50.5 ± 30.2 (± 1σ SD) mg/L, classified as soft water according to the World Health Organization (WHO) classification. The average content of each major component in Japanese tap water tended to be lower than those in other countries. Furthermore, Piper trilinear diagrams were used to categorize Japanese tap water types. The dominating water types were the Ca-HCO3 and mixed types, which had a nationwide distribution. Japanese tap water generally complied with Japanese and WHO drinking water criteria, with only 1% (17/1564 sites) of the samples exceeding water quality standards. Observations of water quality changes for 2 years at three household faucets revealed that fluctuations in major components and trace metals (Al, Fe, Cu, Mn, and Zn) varied in different patterns. This suggests that the behavior of trace metal elements is influenced by local infrastructure, such as supply pipes, distinct from the variability in source water quality.

Low-Cost Sensor Deployment on a Public Minibus in Fukushima Prefecture.

This study analyzed radiation dose data to observe the annual decline in ambient radiation doses and assess the factors contributing to fluctuations in reconstructed areas of the Fukushima prefecture. Utilizing a novel mobile monitoring system installed on a community minibus, the study employed a cost-effective sensor, namely, Pocket Geiger which was integrated with a microcontroller and telecommunication system for data transfer, access, visualization, and accumulation. The study area included the region between Okuma and Tomioka towns. The ambient dose rate recorded along the minibus route was depicted on a map, averaged within a 1 × 1 km mesh created with the Quantum Geographic Information System. To ensure accuracy, the shielding factor of the minibus material is determined to adjust the dose readings. A significant decrease (p < 0.001) in the radiation dose ranges from 2022 to 2023 was observed. The land use classification by the Advanced Land Observation Satellite revealed an ecological half-life ranging from 2.41 years to 1 year, suggesting a rapid radiation decay across all land types. This underscores the close connection between radiation attenuation and environmental factors, as well as decontamination efforts across diverse land categories.

A survey of monitoring tap water hardness in Japan and its distribution patterns.

We conducted a comprehensive overall tap water hardness assessment for Japan. Tap water was collected from 665 points throughout Japan, and its standing position was quantitatively clarified by prefecture. The mean and median hardness of tap water in Japan was 48.9 ± 25.8 (1σ SD) and 46.0 mg/L, respectively. Compared with 27 other countries, Japan exhibited soft water with low-mineral content. Water hardness tended to be high in the Kanto region and low in the Hokkaido and Tohoku regions. The impact of the distribution system's water pipes on tap water hardness is discussed using a unified index to evaluate variations in hardness from raw to tap water. A comparison of the variations in hardness showed that hardness variations from raw to purified water and from purified to tap water exhibited a 20% variation range. Furthermore, tap water hardness and its fluctuations in any region of Japan were found to be caused by raw water hardness. It was demonstrated that the distribution pipe system had no large impacts on water hardness.

Landside tritium leakage over through years from Fukushima Dai-ichi nuclear plant and relationship between countermeasures and contaminated water.

There has been tritium groundwater leakage to the land side of Fukushima Dai-ichi nuclear power plants since 2013. Groundwater was continuously collected from the end of 2013 to 2019, with an average tritium concentration of approximately 20 Bq/L. Based on tritium data published by Tokyo Electric Power Company Holdings (TEPCO) (17,000 points), the postulated source of the leakage was (1) leaks from a contaminated water tank that occurred from 2013 to 2014, or (2) a leak of tritium that had spread widely over an impermeable layer under the site. Based on our results, sea side and land side tritium leakage monitoring systems should be strengthened.

Radioactive Games? Radiation Hazard Assessment of the Tokyo Olympic Summer Games.

We conducted a comprehensive radiation hazard assessment of the Tokyo Olympic Games (Tokyo 2020, postponed to 2021). Our combined experimental and literature study focused on both external and internal exposure to ionizing radiation for athletes and visitors of the Games. The effective dose for a visit of 2 weeks ranges from 57 to 310 µSv (including flight dose). The main contributors to the dose are cosmic radiation during the flights (approximately 10-81%), inhalation of natural radon (approximately 9-47%), and external exposure (approximately 8-42%). In this complex exposure, anthropogenic radionuclides from the Fukushima nuclear accident (2011) always play a minor role and have not caused a significant increase of the radiological risk compared to pre-Fukushima Japan. Significantly elevated air dose rates were not measured at any of the Tokyo Olympic venues. The average air dose rates at the Tokyo 2020 sites were below the average air dose rates at the sites of previous Olympic Games. The level of radiological safety of foods and water is very high in Japan, even for athletes with increased water and caloric demands, respectively.

Radionuclides in surface waters around the damaged Fukushima Daiichi NPP one month after the accident: Evidence of significant tritium release into the environment.

Following the Fukushima nuclear accident (2011), radionuclides mostly of volatile elements (e.g., 131I, 134,137Cs, 132Te) have been investigated frequently for their presence in the atmosphere, pedosphere, biosphere, and the Pacific Ocean. Smaller releases of radionuclides with intermediate volatility, (e.g., 90Sr), have been reported for soil. However, few reports have been published which targeted the contamination of surface (fresh) waters in Japan soon after the accident. In the present study, 10 surface water samples (collected on April 10, 2011) have been screened for their radionuclide content (3H, 90Sr, 129I, 134Cs, and 137Cs), revealing partly unusually high contamination levels. Especially high tritium levels (184 ±â€¯2 Bq·L-1; the highest levels ever reported in scientific literature after Fukushima) were found in a puddle water sample from close to the Fukushima Daiichi nuclear power plant. The ratios between paddy/puddle water from one location only a few meters apart vary around 1% for 134Cs, 12% for 129I (131I), and around 40% for both 3H and 90Sr. This illustrates the adsorption of radiocesium on natural minerals and radioiodine on organic substances (in the rice paddy), whereas the concentration differences of 3H and 90Sr between the two waters are mainly dilution driven.

Source evaluation of 137Cs in foodstuffs based on trace 134Cs radioactivity measurements following the Fukushima nuclear accident.

We performed gamma-ray analysis to determine the amount of radioactive cesium-134 (134Cs) and cesium-137 (137Cs) in 259 foodstuffs five years after the Fukushima nuclear accident of 2011. Using measurements of trace 134Cs radioactivity, we investigated the contribution ratio of 137Cs derived from the Fukushima accident on 2011 and pre-Fukushima. The median detected concentration of radiocesium (134Cs + 137Cs) in foodstuffs was 0.33 Bq/kg-raw, a much lower radioactivity than the Japanese regulatory limit. However, a few samples had particularly high radioactivity, including some dried mushrooms sold in Iwate Prefecture that had a 137Cs radioactivity concentration as high as 441 Bq/kg. Our analysis showed that 75.5% of the 137Cs detected in these mushrooms originated from the Fukushima accident, and 24.5% was originated before the Fukushima event. Our study clarified the 137Cs contamination in 75 of all 259 food samples before and after the Fukushima nuclear accident, showing that not only mushrooms but also fish had been contaminated before the Fukushima accident.

Oxidation of antimony (III) in soil by manganese (IV) oxide using X-ray absorption fine structure.

The oxidation of antimony (III) in soils was studied using X-ray absorption fine structure (XAFS) spectra. An andosol soil sample and artificial soil samples (SiO2 blended with iron (III) hydroxide and manganese (IV) oxide) were used herein. After adding antimony (III) oxide to all soil samples, the oxidation process was observed by recording the XAFS spectra of Sb K-edge, Fe K-edge, and Mn K-edge. The results indicated that manganese (IV) oxide played an important role in the oxidation of Sb(III); however iron (III) hydroxide was not directly related to the reaction. During a 2-hr continuous Sb K-edge X-ray absorption near edge structure (XANES) measurement with an interval of 1min of one of the artificial soil samples (SiO2+MnO2+Sb2O3), a pseudo-first-order reaction was determined with an average estimated rate of 0.52±0.04hr-1. Compared to the lower oxidation rate of andosol, it is suggested that because of the low concentration of Mn(IV) in natural soils, the oxidation process of Sb(III) might be relatively slow and require more time to convert Sb(III) to Sb(V).

Effective and ecological half-lives of 90Sr and 137Cs observed in wheat and rice in Japan.

Published pre-Fukushima food monitoring data from 1963 to 1995 were used to study the long-term presence of 137Cs and 90Sr in rice and wheat. Effective half-lives (Teff) were calculated for rice (137Cs: 5.6 years; 90Sr: 6.7 years) and wheat (137Cs: 3.5 years; 90Sr: 6.2 years), respectively. In rice, 137Cs exhibits a longer Teff because putrefaction processes will lead to the formation of NH4+ ions that are efficient ion exchangers for mineral-adsorbed cesium ions, hence making it more readily available to the plant. Knowledge on the long-term behavior of radiocesium and radiostrontium will be important for Japanese food-safety campaigns after the Fukushima nuclear accident.

Fukushima-derived radionuclides in sediments of the Japanese Pacific Ocean coast and various Japanese water samples (seawater, tap water, and coolant water of Fukushima Daiichi reactor unit 5).

We investigated Ocean sediments and seawater from inside the Fukushima exclusion zone and found radiocesium (134Cs and 137Cs) up to 800 Bq kg-1 as well as 90Sr up to 5.6 Bq kg-1. This is one of the first reports on radiostrontium in sea sediments from the Fukushima exclusion zone. Seawater exhibited contamination levels up to 5.3 Bq kg-1 radiocesium. Tap water from Tokyo from weeks after the accident exhibited detectable but harmless activities of radiocesium (well below the regulatory limit). Analysis of the Unit 5 reactor coolant (finding only 3H and even low 129I) leads to the conclusion that the purification techniques for reactor coolant employed at Fukushima Daiichi are very effective.

Post-Accident Sporadic Releases of Airborne Radionuclides from the Fukushima Daiichi Nuclear Power Plant Site.

The Fukushima nuclear accident (March 11, 2011) caused the widespread contamination of Japan by direct deposition of airborne radionuclides. Analysis of weekly air filters has revealed sporadic releases of radionuclides long after the Fukushima Daiichi reactors were stabilized. One major discharge was observed in August 2013 in monitoring stations north of the Fukushima Daiichi nuclear power plant (FDNPP). During this event, an air monitoring station in this previously scarcely contaminated area suddenly reported (137)Cs activity levels that were 30-fold above the background. Together with atmospheric dispersion and deposition simulation, radionuclide analysis in soil indicated that debris removal operations conducted on the FDNPP site on August 19, 2013 are likely to be responsible for this late release of radionuclides. One soil sample in the center of the simulated plume exhibited a high (90)Sr contamination (78 ± 8 Bq kg(-1)) as well as a high (90)Sr/(137)Cs ratio (0.04); both phenomena have usually been observed only in very close vicinity around the FDNPP. We estimate that through the resuspension of highly contaminated particles in the course of these earthmoving operations, gross (137)Cs activity of ca. 2.8 × 10(11) Bq has been released.

Detection of fuel release in a nuclear accident: a method for preconcentration and isolation of reactor-borne (239)Np using ion-specific extraction chromatography.

Although actinides are the most informative elements with respect to the nature of a nuclear accident, plutonium analysis is complicated by the background created by fallout from atmospheric nuclear explosions. Therefore, we propose (239)Np, a short-lived actinide that emits several γ rays, as a preferred proxy. The aim of this study was to screen ion specific extraction chromatography resins (RE-, TEVA-, UTEVA-, TRU-, and Actinide-Resin) for the highest possible recovery and separation of trace amounts of (239)Np from samples with large activities of fission products such as radiocesium, radioiodine, and, most importantly, radiotellurium, the latter of which causes spectral interference in gamma spectrometry through overlapping peaks with (239)Np. The investigated environmental media for these separations were aqueous solutions simulating rainwater and soil. Spiked samples containing (239)Np and the aforementioned volatile radionuclides were separated through extraction chromatographic columns to ascertain the most effective means of separating (239)Np from other fission products for detection by gamma spectroscopy. We propose a method for nuclear accident preparedness based on the use of Eichrom's RE-Resin. The proposed method was found most effective for isolating (239)Np from interfering radionuclides in both aqueous solution and soil using 8 M HNO3 as the loading solution and H2O as the eluent. The RE-Resin outperforms the more commonly used TEVA-Resin because the TEVA-Resin showed a higher affinity for interfering radiotellurium and radioiodine.

Analysis of Japanese radionuclide monitoring data of food before and after the Fukushima nuclear accident.

In an unprecedented food monitoring campaign for radionuclides, the Japanese government took action to secure food safety after the Fukushima nuclear accident (Mar. 11, 2011). In this work we analyze a part of the immense data set, in particular radiocesium contaminations in food from the first year after the accident. Activity concentrations in vegetables peaked immediately after the campaign had commenced, but they decreased quickly, so that by early summer 2011 only a few samples exceeded the regulatory limits. Later, accumulating mushrooms and dried produce led to several exceedances of the limits again. Monitoring of meat started with significant delay, especially outside Fukushima prefecture. After a buildup period, contamination levels of meat peaked by July 2011 (beef). Levels then decreased quickly, but peaked again in September 2011, which was primarily due to boar meat (a known accumulator of radiocesium). Tap water was less contaminated; any restrictions for tap water were canceled by April 1, 2011. Pre-Fukushima (137)Cs and (90)Sr levels (resulting from atmospheric nuclear explosions) in food were typically lower than 0.5 Bq/kg, whereby meat was typically higher in (137)Cs and vegetarian produce was usually higher in (90)Sr. The correlation of background radiostrontium and radiocesium indicated that the regulatory assumption after the Fukushima accident of a maximum activity of (90)Sr being 10% of the respective (137)Cs concentrations may soon be at risk, as the (90)Sr/(137)Cs ratio increases with time. This should be taken into account for the current Japanese food policy as the current regulation will soon underestimate the (90)Sr content of Japanese foods.

Reduction process of Cr(VI) by Fe(II) and humic acid analyzed using high time resolution XAFS analysis.

The initial reduction behavior of Cr(VI) to Cr(III) has not been clearly understood due to its rapid reduction reaction. In order to study the reduction process of Cr(VI) in detail, we applied quick X-ray absorption fine structure (QXAFS) analysis to observe how Cr(VI) was reduced to Cr(III) by Fe(II) and humic acid (HA) with time. The Cr(VI) concentration was analyzed every 60s, and the plots of ln(Cr(VI)/Cr(VI)0) versus time were used to evaluate the reduction process based on their linearity. Reduction by Fe(II) showed a linear relation, whereas reduction by HA showed a nonlinear relation. With combined Fe(II) and HA, the linearity was unlike those of Fe(II) and HA individually. The reduction rate was not constant. The structure of Fe(II) produced by HA during the Cr(VI) reduction was investigated by using Mössbauer spectroscopy, which showed that Fe(II) produced by HA reduction of Fe(III) had the same structure as the initial Fe(II). HA can reduce Fe(III) back to Fe(II), and reproduced Fe(II) reduces Cr(VI). For Cr(VI) reduction by combined Fe(II) and HA, each reductant contribute differently: Fe(II) directly contributes to the Cr(VI) reaction, whereas HA reduces both Cr(VI) and Fe(III).

Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations.

The contamination of Japan after the Fukushima accident has been investigated mainly for volatile fission products, but only sparsely for actinides such as plutonium. Only small releases of actinides were estimated in Fukushima. Plutonium is still omnipresent in the environment from previous atmospheric nuclear weapons tests. We investigated soil and plants sampled at different hot spots in Japan, searching for reactor-borne plutonium using its isotopic ratio ²4°Pu/²³9Pu. By using accelerator mass spectrometry, we clearly demonstrated the release of Pu from the Fukushima Daiichi power plant: While most samples contained only the radionuclide signature of fallout plutonium, there is at least one vegetation sample whose isotope ratio (0.381 ± 0.046) evidences that the Pu originates from a nuclear reactor (²³9⁺²4°Pu activity concentration 0.49 Bq/kg). Plutonium content and isotope ratios differ considerably even for very close sampling locations, e.g. the soil and the plants growing on it. This strong localization indicates a particulate Pu release, which is of high radiological risk if incorporated.

Concentration of strontium-90 at selected hot spots in Japan.

This study is dedicated to the environmental monitoring of radionuclides released in the course of the Fukushima nuclear accident. The activity concentrations of ß(-)-emitting (90)Sr and ß(-)/γ-emitting (134)Cs and (137)Cs from several hot spots in Japan were determined in soil and vegetation samples. The (90)Sr contamination levels of the samples were relatively low and did not exceed the Bq⋅g(-1) range. They were up four orders of magnitude lower than the respective (137)Cs levels. This study, therefore, experimentally confirms previous predictions indicating a low release of (90)Sr from the Fukushima reactors, due to its low volatility. The radiocesium contamination could be clearly attributed to the Fukushima nuclear accident via its activity ratio fingerprint ((134)Cs/(137)Cs). Although the correlation between (90)Sr and (137)Cs is relatively weak, the data set suggests an intrinsic coexistence of both radionuclides in the contaminations caused by the Fukushima nuclear accident. This observation is of great importance not only for remediation campaigns but also for the current food monitoring campaigns, which currently rely on the assumption that the activity concentrations of ß(-)-emitting (90)Sr (which is relatively laborious to determine) is not higher than 10% of the level of γ-emitting (137)Cs (which can be measured quickly). This assumption could be confirmed for the samples investigated herein.

Deposition of fission and activation products after the Fukushima Dai-ichi nuclear power plant accident.

The Great Eastern Japan Earthquake on March 11, 2011, damaged reactor cooling systems at Fukushima Dai-ichi nuclear power plant. The subsequent venting operation and hydrogen explosion resulted in a large radioactive nuclide emission from reactor containers into the environment. Here, we collected environmental samples such as soil, plant species, and water on April 10, 2011, in front of the power plant main gate as well as 35 km away in Iitate village, and observed gamma-rays with a Ge(Li) semiconductor detector. We observed activation products ((239)Np and (59)Fe) and fission products ((131)I, (134)Cs ((133)Cs), (137)Cs, (110m)Ag ((109)Ag), (132)Te, (132)I, (140)Ba, (140)La, (91)Sr, (91)Y, (95)Zr, and (95)Nb). (239)Np is the parent nuclide of (239)Pu; (59)Fe are presumably activation products of (58)Fe obtained by corrosion of cooling pipes. The results show that these activation and fission products, diffused within a month of the accident.