Tissue-free water tritium and non-exchangeable organically bound tritium concentrations in fish near coastline during and after operation of Japan's first nuclear fuel reprocessing facility.

The risks from radioactive wastewater release from nuclear facilities into the ocean are a global concern. Radioactive contaminants, such as tritium (3H), in both forms of tissue free water tritium (TFWT) and non-exchangeable organically bound tritium (NE-OBT), can be incorporated into marine biota and cause radiation doses to biota and future consumers. However, no studies have been conducted to measure both forms of 3H in marine fish as well as evaluate the residence time in the vicinity of a nuclear fuel reprocessing facility. Here, fish from a brackish lake and from the Pacific Ocean coastline of Japan, which are near such a facility, were collected between 2006 and 2021. The reprocessing facility was operational between 2006 and 2009, during which time about 300 times more tritiated water was discharged per year into the ocean compared to the period when the facility was not operational. During operation the annual release was 30 times higher than the treated water released annually from Fukushima Daiichi. As expected, TFWT and NE-OBT concentrations increased in marine fish during operations and had peak values of 3.59 ±â€¯0.03 and 0.56 ±â€¯0.03 Bq/L, respectively. Total dose rates to the fish were 36,000 times lower than the 10 µGy h-1 benchmark. Concentrations gradually decreased to pre-operational levels as the facility was turned off with NE-OBT taking twice as long. Fish sampled from the brackish lake tended to have more incorporated TFWT and NE-OBT concentrations than ocean fish. This indicates that ocean tides might have contributed to the accumulation of discharged tritiated water in the lake via a narrow water channel, which highlights the importance of examining all marine ecosystems in future operations. In both marine environments, the estimated committed effective dose using the highest observed data through ingestion was well below public limits (91,000 times lower).

Variation analysis of atmospheric 7Be activity concentrations with respect to precipitation.

Beryllium-7 activity concentrations in the atmosphere and precipitation were continuously measured every day between April 2011 and December 2015 in Dazaifu, western Japan. The measured data were quantitatively analyzed to determine the precipitation-induced variation in 7Be activity concentrations. The average concentrations on nonprecipitation and precipitation days were 5.5 and 3.8 mBq/m3, respectively. This difference of 31% (1.7 mBq/m3) on average, was attributable to the washout effect, which was more significant in the summer. Regarding the association between 7Be activity concentration and precipitation, the concentration remained at a similar level for the small precipitation amount of <5.0 mm/day and showed a decreasing trend (but was insignificant) for the precipitation of 5.0-10.0 mm/day. A significant decrease in the concentration was observed for ≥10 mm/day. Furthermore, when precipitation occurred on two successive days, the 7Be activity concentrations on the second day significantly decreased regardless of precipitation.

Temporal variation of tritium concentration in monthly precipitation collected at a Difficult-to-Return Zone in Namie Town, Fukushima Prefecture, Japan.

This article discusses tritium concentrations in monthly precipitation in part of the Difficult-to-Return Zone in Namie Town during 2012-2021. The tritium concentrations, which were measured with a low background liquid scintillation counter after carrying out an enrichment procedure, fluctuated seasonally from 0.10 ± 0.02 to 0.85 ± 0.02 Bq L-1. This range of concentrations is concluded to not be unusual based on comparisons with the concentrations at other sites and estimates of the past range of the concentrations. Moreover, no significant variations in observed tritium concentrations were observed due to decommissioning work at the Fukushima Dai-ichi Nuclear Power Plant. These results contribute to understanding the background level of tritium concentration in precipitation before the oceanic discharge of treated water from the Fukushima plant. In addition, this article evaluates the amount of tritium supplied to the ocean by terrestrial rainwater pouring into the Pacific Ocean via Ukedo River, which flows through Namie Town; this information will contribute to the discussion on the impact of the oceanic discharge of treated water.

Calibration experiments for radon in drinking water measurements using portable-type electrostatic-collection radon monitors.

Portable-type electrostatic-collection radon monitors (RAD7) are often used for in-situ measurements of radon in water. In this study, we evaluated the calibration factors and their uncertainties for two RAD7 monitors based on comparative measurements with the liquid scintillation counting method. In the first experiment, we found that both RAD7 monitors had relatively large uncertainties due to leakage of radon gas that bubbled from the gaps between the lids of the desiccant container and the glass vial. Therefore, for the second experiment, these gaps were closed as much as possible using parafilm and clay, respectively. As a result, the relative uncertainties for both RAD7 monitors were significantly decreased. Furthermore, we collected spring water samples to confirm the reliability of radon concentrations. After closing the leakage point, the uncertainty of radon concentrations in spring water we measured using the typical protocol of the RAD7 were significantly lower, which improves the measurement.

SPECIATION OF CESIUM ISOTOPES IN RIVER WATER: A CASE STUDY IN THE UKEDO RIVER.

137Cs in river systems can be taken up by aquatic animals. In this paper, total 137Cs concentration in the Ukedo River system and 137Cs presence in dissolved, acid-soluble and -insoluble fractions in river water samples were determined. Total 137Cs concentration had the maximum value of 2.08 Bq kg-1 below the Ogaki Dam in May 2012. In the base flow condition, > 87% of 137Cs existed in the dissolved state, and the acid-soluble state and the insoluble state were <13% and the undetectable level, respectively. After the heavy rain event, the particulate fraction (acid-soluble state + insoluble state) was elevated to 65%, which corresponds to twice as much as that in the base flow condition. Particulate 137Cs, especially the acid-soluble Cs, can play a role when taken into the food chain in aquatic ecosystems.

INFLUENCE OF SAMPLING FLOW RATE ON THORON EXHALATION RATE MEASUREMENTS BY THE CIRCULATION METHOD.

Researchers have used various methods to obtain the exhalation rates of radon and thoron from soil and building materials. One of the typical methods for radon exhalation rate is the circulation method using an accumulation container, an external or internal sampling pump and a continuous radon monitor. However, it is necessary to consider sampling flow rate if this method is applied to exhalation rate measurement for thoron due to its short half-life. Based on a calibration experiment, the measured thoron concentrations obtained by an electrostatic collection type radon and thoron monitor (RAD7) were found to be influenced strongly by the sampling flow rate. It was also found that the thoron exhalation rate from a soil sample depended on the pressure difference which was proportional to the increasing sampling flow rate. The thoron exhalation rate measured at the generally used sampling flow rate of the internal sampling pump of the RAD7 was overestimated compared with the value at 0 L min-1.

TRITIUM CONCENTRATION IN MONTHLY PRECIPITATION NEAR THE FUSION TEST FACILITY IN JAPAN BEFORE AND AFTER THE DEUTERIUM PLASMA EXPERIMENT.

In Japan, the deuterium plasma experiment using the Large Helical Device was started at the National Institute for Fusion Science (NIFS) in March 2017 to investigate high-temperature plasma physics and hydrogen isotope effects in research leading towards the realisation of fusion energy. The deuterium plasma experiment produces small amount of tritium by fusion reactions. To understand any impacts by the experiment to the surrounding environment, monthly precipitation samples have been collected at the NIFS site since November 2013 to assess the relationship between isotope composition and chemical species in precipitation including tritium. By comparing data before and after the deuterium plasma experiment start, it was found that tritium released from the main stack of the fusion test facility had no impact on the environment surrounding NIFS.

PERFORMANCE EVALUATION OF COMMERCIAL SCINTILLATION COCKTAILS FOR LOW-LEVEL TRITIUM COUNTING BY HIGH-CAPACITY LIQUID SCINTILLATION COUNTER.

Low-background liquid scintillation counter is one of the popular measuring instruments used to investigate tritium radioactivity in environmental media. These instruments require the liquid sample and organic solvent to be mixed for tritium measurement. In the European Union, the registration, evaluation, authorization and restriction of chemicals regulation was established to control the use of chemical substances of very high concern. It is important to find continuously available alternative reagents. In this paper, a performance evaluation was conducted using four scintillation cocktails according to Japanese conventional procedure; although one of them, Gold Star LT2, contains nonylphenol ethoxylate, it will continue to be available for research and development. From the evaluation results it was confirmed that Gold Star LT2 would be a satisfactory alternative scintillator, which is similar performance of Ultima Gold LLT.

LEVELS OF ATMOSPHERIC TRITIUM IN THE SITE OF FUSION TEST FACILITY.

In the deuterium plasma experiment using Large Helical Device at the National Institute for Fusion Science (NIFS), a small amount of tritium is produced by the D-D fusion reaction. Then, a part of produced tritium is discharged into the environment via a stack. Thus, the atmospheric tritium in the site of NIFS has been monitored before starting the deuterium plasma experiment. The atmospheric tritium concentrations at NIFS were indicated to be background levels in Japan. To investigate the impact of tritium discharged from the stack, the correlation between the atmospheric tritium concentration and the tritium concentration observed in the stack was evaluated, and no significant correlation was found. In addition, the atmospheric tritium concentration at NIFS ranged within the background levels in Japan. Therefore, the impact of discharged tritium from the stack would be negligible in the environment at NIFS.

TEMPORAL VARIATION OF POST-ACCIDENT 129I IN ATMOSPHERIC PARTICULATE MATTER COLLECTED FROM AN EVACUATED AREA OF FUKUSHIMA PREFECTURE, JAPAN.

To understand the behavior of atmospheric 129I that originated from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident, activity concentrations of 129I in samples of atmospheric particulate matter (PM), comprising coarse (>1.1 µm) and fine (<1.1 µm) fractions (separated using a single stage impactor), were measured on a nearly monthly basis from October 2012 to October 2014 at a site in an area evacuated after the FDNPP accident. Total atmospheric 129I activity concentrations in PM at the site ranged between 0.15 and 2.17 nBq m-3. Specific activity concentration of 129I in total atmospheric PM ranged between 40.8 and 336 mBq kg-1, with a mean and standard deviation of 142 and 77.6 mBq kg-1, respectively. The specific activity in PM tended to be higher than not only the background values reported from soil collected before the FDNPP accident but also than those reported from the contaminated soil after the accident (range: 1.6-57 mBq kg-1; mean and standard deviation: 10.6 and 12.3 mBq kg-1, respectively). Total 129I/127I atomic ratios in PM ranged from 2.0 × 10-8 to 59.8 × 10-8, with a mean and standard deviation of 15.0 × 10-8 and 14.4 × 10-8, respectively. These ratios were generally lower than those of the contaminated soil collected after the FDNPP accident (range: 4.9 × 10-8-443 × 10-8; mean and standard deviation: 74.2 × 10-8 and 85.4 × 10-8, respectively). The 129I concentration and 129I/127I atomic ratio in atmospheric PM showed different characteristics from that of contaminated soils, suggesting that the presence of other atmospheric PMs plays a more important role as the host for 129I.

Analysis of Factors Contributing to the Increase in 7Be Activity Concentrations in the Atmosphere.

In March 2013, increased 7Be activity concentrations in the atmosphere were observed for successive days in Dazaifu, western Japan. The daily 7Be activity concentration ranged from 0.93 to 14 mBq/m3, with a monthly average of 8.3 mBq/m3. This average was the highest among the monthly averages observed between 1999 and 2015, and higher than the monthly average over this period (4.7 mBq/m3) plus twice the standard deviation. Also, this exceeded the monthly average (6.0 mBq/m3) only for March 1999-2015 (excluding 2013, when the cosmic-ray intensity, a component producing 7Be, decreased). Based on the backward trajectory analysis etc. results, the inflow of air from the stratosphere and upper troposphere at high latitudes that frequently occurred in March 2013 was considered the reason for the 7Be activity concentration increase.

222Rn and 226Ra Concentrations in Spring Water and Their Dose Assessment Due to Ingestion Intake.

222Rn and 226Ra concentrations of less than a few to several thousands of Bq L-1 have been observed in several underground bodies of water around the world. Although regulations for these concentrations in water have been implemented internationally, there are currently no regulations in place in Japan. However, concentrations that exceed these internationally recognized regulatory values have also been observed in Japan. In this study, concentrations in spring water in the northern part of Japan were measured and the effective dose from intake of the water was evaluated. 222Rn concentrations were measured using a liquid scintillation counter, and 226Ra concentrations were measured using a high purity germanium detector after chemical preparation. The measured 222Rn concentrations (=12.7 ± 6.1 Bq L-1) and 226Ra concentrations (<0.019-0.022 Bq L-1) did not exceed the reference values set by international and European/American organizations. A conservative estimate of the annual effective ingestion dose of 8 µSv for 222Rn and 226Ra obtained in this study is much smaller than the estimated overall annual effective dose of 2.2 mSv from natural radiation to the Japanese population. However, this dosage accounts for 8% of the WHO individual dosing criteria of 0.1 mSv/year for drinking water.

Heavy Metal Assessments of Soil Samples from a High Natural Background Radiation Area, Indonesia.

Mamuju, Indonesia, is an area with high natural background radiation. This study assesses heavy metal content in soil samples from this area to determine the level of public and environmental hazard it presents. This study analyzes natural radionuclide elements using high purity germanium (HPGe) gamma spectrometry and performs heavy metals analysis using a flame atomic absorption spectrometry (FAAS). Moreover, pollution indices and descriptive analyses were used to assess heavy metal contamination in the environment and the correlation between heavy metals and radionuclides. The results demonstrate that soil samples in several areas of Mamuju contain a high concentration of the natural radionuclides 226Ra and 232Th, and that heavy metal concentrations in the soil decrease in the sequence Zn > Pb > Cr > Cu > Ni > Cd. This study revealed that soil samples from Mamuju are moderately contaminated. There was a strong positive relationship between 226Ra, 232Th, ambient dose equivalent rate, and Pb. Ecological risk index (RI) and cumulative pollution index (IPI) values in Mamuju are 2.05 and 125, respectively, which are possible hazards to human health as a result. Pb concentration in the Mamuju soil samples ranged from 109 to 744 mg kg-1, exceeding the worldwide average of 27 mg kg-1.

Comprehensive exposure assessments from the viewpoint of health in a unique high natural background radiation area, Mamuju, Indonesia.

Mamuju is one of the regions in Indonesia which retains natural conditions but has relatively high exposure to natural radiation. The goals of the present study were to characterize exposure of the entire Mamuju region as a high natural background radiation area (HNBRA) and to assess the existing exposure as a means for radiation protection of the public and the environment. A cross-sectional study method was used with cluster sampling areas by measuring all parameters that contribute to external and internal radiation exposures. It was determined that Mamuju was a unique HNBRA with the annual effective dose between 17 and 115 mSv, with an average of 32 mSv. The lifetime cumulative dose calculation suggested that Mamuju residents could receive as much as 2.2 Sv on average which is much higher than the average dose of atomic bomb survivors for which risks of cancer and non-cancer diseases are demonstrated. The study results are new scientific data allowing better understanding of health effects related to chronic low-dose-rate radiation exposure and they can be used as the main input in a future epidemiology study.

Support activities in Namie Town, Fukushima undertaken by Hirosaki University.

This paper does not necessarily reflect the views of the International Commission on Radiological Protection.Several radiation monitoring research projects are underway on dose assessment, biological analysis, and risk communication under an agreement with Namie Town. Indoor radon and thoron progeny concentrations have been measured using passive-type monitors to estimate internal doses due to inhalation. In addition, airborne radiocaesium concentrations at five points in Namie Town have been analysed using a high-purity germanium detector to estimate internal doses for comparison with radon. External radiation doses from natural and artificial radionuclides have also been estimated using an in-situ gamma-ray spectrometer. Other support activities are mentioned briefly in this article.

Long-Term Measurements of Radon and Thoron Exhalation Rates from the Ground Using the Vertical Distributions of Their Activity Concentrations.

A long-term measurement technique of radon exhalation rate was previously developed using a passive type radon and thoron discriminative monitor and a ventilated type accumulation chamber. In the present study, this technique was applied to evaluate the thoron exhalation rate as well, and long-term measurements of radon and thoron exhalation rates were conducted for four years in Gifu Prefecture. The ventilated type accumulation chamber (0.8 × 0.8 × 1.0 m3) with an open bottom was embedded 15 cm into the ground. The vertical distributions of radon and thoron activity concentrations from the ground were obtained using passive type radon-thoron discriminative monitors (RADUETs). The RADUETs were placed at 1, 3, 10, 30, and 80 cm above the ground inside the accumulation chamber. The measurements were conducted from autumn 2014 to autumn 2018. These long-term results were found to be in good agreement with the values obtained by another methodology. The radon exhalation rates from the ground showed a clearly seasonal variation. Similar to findings of previous studies, radon exhalation rates from summer to autumn were relatively higher than those from winter to spring. In contrast, thoron exhalation rates were not found to show seasonal variation.

Temporal and Spatial Variation of Radon Concentrations in Environmental Water from Okinawa Island, Southwestern Part of Japan.

In this study, to get a better understanding in characterizing groundwater and ensure its effective management, the radon concentrations in water samples were measured through Ryukyu limestone in southern Okinawa Island, Japan. Water samples were collected from a limestone cave (Gyokusendo cave, dropping water) and two springs (Ukinju and Komesu, spring water), and the radon concentrations were measured by liquid scintillation counters. The radon concentrations in the samples from the Gyokusendo cave, and Ukinju and Komesu springs were 10 ± 1.3 Bq L-1, 3.2 ± 1.0 Bq L-1, and 3.1 ± 1.1 Bq L-1, respectively. The radon concentrations showed a gradually increasing trend from summer to autumn and decreased during winter. The variation of radon concentrations in the dripping water sample from the Gyokusendo cave showed a lagged response to precipitation changes by approximately 2-3 months. The estimated radon concentrations in the dripping water sample were calculated with the measured radon concentrations from the dripping water obtained during the study period. Based on our results, groundwater in the Gyokusendo cave system was estimated to percolate through the Ryukyu limestone in 7-10 days, and the residence time of groundwater in the soil above Gyokusendo cave was estimated to be approximately 50-80 days. This work makes a valuable contribution to the understanding of groundwater processes in limestone aquifers, which is essential for ensuring groundwater sustainability.

Discriminative Measurement of Absorbed Dose Rates in Air from Natural and Artificial Radionuclides in Namie Town, Fukushima Prefecture.

Ten years have elapsed since the accident at the Fukushima Daiichi Nuclear Power Plant in 2011, and the relative contribution of natural radiation is increasing in Fukushima Prefecture due to the reduced dose of artificial radiation. In order to accurately determine the effective dose of exposure to artificial radiation, it is necessary to evaluate the effective dose of natural as well as artificial components. In this study, we measured the gamma-ray pulse-height distribution over the accessible area of Namie Town, Fukushima Prefecture, and evaluated the annual effective dose of external exposure by distinguishing between natural and artificial radionuclides. The estimated median (range) of absorbed dose rates in air from artificial radionuclides as of 1 April 2020, is 133 (67-511) nGy h-1 in the evacuation order cancellation zone, and 1306 (892-2081) nGy h-1 in the difficult-to-return zone. The median annual effective doses of external exposures from natural and artificial radionuclides were found to be 0.19 and 0.40 mSv in the evacuation order cancellation zone, and 0.25 and 3.9 mSv in the difficult-to-return zone. The latest annual effective dose of external exposure discriminated into natural and artificial radionuclides is expected to be utilized for radiation risk communication.

A unique high natural background radiation area - Dose assessment and perspectives.

The biological effects of low dose-rate radiation exposures on humans remains unknown. In fact, the Japanese nation still struggles with this issue after the Fukushima Dai-ichi Nuclear Power Plant accident. Recently, we have found a unique area in Indonesia where naturally high radiation levels are present, resulting in chronic low dose-rate radiation exposures. We aimed to estimate the comprehensive dose due to internal and external exposures at the particularly high natural radiation area, and to discuss the enhancement mechanism of radon. A car-borne survey was conducted to estimate the external doses from terrestrial radiation. Indoor radon measurements were made in 47 dwellings over three to five months, covering the two typical seasons, to estimate the internal doses. Atmospheric radon gases were simultaneously collected at several heights to evaluate the vertical distribution. The absorbed dose rates in air in the study area vary widely between 50 nGy h-1 and 1109 nGy h-1. Indoor radon concentrations ranged from 124 Bq m-3 to 1015 Bq m-3. That is, the indoor radon concentrations measured exceed the reference levels of 100 Bq m-3 recommended by the World Health Organization. Furthermore, the outdoor radon concentrations measured were comparable to the high indoor radon concentrations. The annual effective dose due to external and internal exposures in the study area was estimated to be 27 mSv using the median values. It was found that many residents are receiving radiation exposure from natural radionuclides over the dose limit for occupational exposure to radiation workers. This enhanced outdoor radon concentration might be as a result of the stable atmospheric conditions generated at an exceptionally low altitude. Our findings suggest that this area provides a unique opportunity to conduct an epidemiological study related to health effects due to chronic low dose-rate radiation exposure.

CAESIUM RETENTION CHARACTERISTICS OF KNIFC-PAN RESIN FROM RIVER WATER.

The caesium retention characteristics of a potassium-nickel hexacyanoferrate resin in a polyacrylnitrile (KNiFC-PAN) matrix were tested in fresh water over the range of 2.5-400 mL min-1. The experimental setup used 2 mL resin and 4-L aliquots of freshwater samples. The results showed nearly 100% retention at speeds below 10 mL min-1, above 80% up to 100 mL min-1, and approached 50% at 400 mL min-1. Using 100 mL min-1 flow rate and KNiFC-PAN resin in a well-type HPGe detector, the minimum detectable concentration was reduced to 3 mBq kg-1 for 4-L aliquots of water samples from the previous 15 mBq kg-1 achieved by Powdex ion-exchange resin and a planar type HPGe detector.