Distribution of naturally occurring radionuclides and gamma dose rate assessment in the soils of high background natural radiation area Odisha, India.

A study on the activity concentration of primordial radionuclides 226Ra, 232Th and 40K was carried out on the surface soil samples collected from the coastal villages between Chhatrapur and Gopalpur regions of high background natural radiation area Odisha, India, using high purity germanium gamma spectroscopy. The mean activity concentrations of 226Ra, 232Th and 40K were found to be 231, 1692 and 250 Bq/kg, respectively. The total mean absorbed dose owing to the presence of 226Ra, 232Th and 40K was 1139 nGy/h. The mean annual effective dose was found to be 1397 µSv/y and higher than the UNSCEAR average value 70 µSv/y.

234U/238U disequilibrium and 235U/238U ratios measured using MC-ICP-MS in natural high background radiation area soils to understand the fate of uranium.

The Chhatrapur-Gopalpur coastal area in Odisha, India is a well-known natural high background radiation (HBRA) area due to the abundance of monazite (a thorium bearing radioactive mineral) in beach sands and soils. Recent studies on Chhatrapur-Gopalpur HBRA groundwater have reported high concentrations of uranium and its decay products. Therefore, the soils of the Chhatrapur-Gopalpur HBRA are reasonably suspected as the sources of these high uranium concentrations in groundwater. In this report, first the uranium concentrations in soil samples were measured using inductively coupled plasma mass spectrometry (ICP-MS) and they were found to range from 0.61 ± 0.01 to 38.59 ± 0.16 mg kg-１. Next, the 234U/238U and 235U/238U isotope ratios were measured to establish a baseline for the first time in Chhatrapur-Gopalpur HBRA soil. Multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) was used for measurement of these isotope ratios. The 235U/238U ratio was observed to be the normal terrestrial value. The 234U/238U activity ratio, was calculated to understand the secular equilibrium between 234U and 238U in soil and it varied from 0.959 to 1.070. To understand the dynamics of uranium in HBRA soil, physico-chemical characteristics of soil were correlated with uranium isotope ratios and this correlation of 234U/238U activity ratio indicated the leaching of 234U from Odisha HBRA soil.

DISTRIBUTION OF RADIOCESIUM CONCENTRATIONS OF SOILS IN THE EIGHT IZU ISLANDS AFTER THE FUKUSHIMA DAIICHI NUCLEAR POWER PLANT ACCIDENT.

Large amounts of anthropogenic radionuclides, such as 134Cs and 137Cs(radiocesium), were released into the atmosphere due to the Fukushima Daiichi Nuclear Power Plant (F1-NPP) accident and were transported into various environments. The soil accumulations of diffused radionuclides are marked by large differences in their horizontal distributions, and the vertical air dose rates vary depending on the topography, altitude and other factors. In this study, soil activity concentrations of eight islands in the Izu Islands, ~334-563 km south of the F1-NPP, were analyzed from both horizontal and vertical perspectives. Soil samples were collected over a 4-y period from 2012 to 2016, and their activity concentrations of radiocesium were measured. The activity concentrations in the soil were categorized for intervals of a 100-m altitude above sea level, and the relationship between the maximum activity concentration in each category and the distance from the F1-NPP was analyzed. The correlation was good at the lower altitudes.

Measurements and future projections of Gd-based contrast agents for MRI exams in wastewater treatment plants in the Tokyo metropolitan area.

Large amounts of Gd-based contrast agents are used in magnetic resonance imaging (MRI) that are then excreted in urine. These agents are subsequently discharged into the environment because they are difficult to remove by usual sewage treatment techniques. In this study, changes of the Gd anomaly during wastewater treatment processes were determined by analyzing wastewater samples and the possibility for future prediction of the changes was evaluated based on the relationship between the Gd anomaly and the number of MRI devices in use. After the wastewater treatment processes, the values of final effluent were increased 1.8 times compared to those of influent, and the Gd anomaly of effluent had a positive correlation to the number of MRI devices. The finding suggested that the changes of environmental impact were predictable based on the number of MRI devices.

ICP-MS Measurement of Trace and Rare Earth Elements in Beach Placer-Deposit Soils of Odisha, East Coast of India, to Estimate Natural Enhancement of Elements in the Environment.

Inductively coupled plasma mass spectrometry (ICP-MS) has been used to measure the concentration of trace and rare earth elements (REEs) in soils. Geochemical certified reference materials such as JLk-1, JB-1, and JB-3 were used for the validation of the analytical method. The measured values were in good agreement with the certified values for all the elements and were within 10% analytical error. Beach placer deposits of soils mainly from Odisha, on the east coast of India, have been selected to study selected trace and rare earth elements (REEs), to estimate enrichment factor (EF) and geoaccumulation index (Igeo) in the natural environment. Enrichment factor (EF) and geoaccumulation index (Igeo) results showed that Cr, Mn, Fe, Co, Zn, Y, Zr, Cd and U were significantly enriched, and Th was extremely enriched. The total content of REEs (Æ©REEs) ranged from 101.3 to 12,911.3 µg g-1, with an average 2431.1 µg g-1 which was higher than the average crustal value of ΣREEs. A high concentration of Th and light REEs were strongly correlated, which confirmed soil enrichment with monazite minerals. High ratios of light REEs (LREEs)/heavy REEs (HREEs) with a strong negative Eu anomaly revealed a felsic origin. The comparison of the chondrite normalized REE patterns of soil with hinterland rocks such as granite, charnockite, khondalite and migmatite suggested that enhancement of trace and REEs are of natural origin.

Geochemical behavior of uranium and thorium in sand and sandy soil samples from a natural high background radiation area of the Odisha coast, India.

Owing to their natural radioactivity, uranium (U) and thorium (Th) play significant roles in environmental sciences for monitoring radiation dose and in geological sciences for understanding sedimentary processes. The Odisha coastal area, in eastern India, is a well-known high background radiation area that is rich in monazites and rutile. This area was selected to study geochemical characteristics of U and Th in sand and sandy soil samples. The concentrations of U and Th were measured using inductively coupled plasma mass spectrometry (ICP-MS). The median, geometric mean, and standard deviation for U were determined to be 6, 4.5, and 2.5 µg/g and for Th were 186, 123.3, and 3.1 µg/g, respectively. Major element concentrations were evaluated using X-ray fluorescence spectroscopy to get the mineralogical composition and state of chemical weathering. The ratios of Th/U and Th/K varied from 4 to 37 and from 13 to 1058, respectively. These results clearly indicate that the samples from the coastal region were formed in an oxidizing and intense chemical weathering terrestrial environment with an enrichment of radiogenic heavy minerals (monazites and zircon) and clay mineral association. Since the majority of the samples have undergone moderate to intense weathering in the oxidizing environment, U is leached from the soil and sand matrix. Eventually, Th resides in the matrix and becomes a major source for radiation exposure in the environment. The high ratios of Th/U, along with the strong positive correlation between Th and P2O5, evidence the enrichment of the Th-bearing radioactive mineral, monazite, in these samples.

Chemical Separation of Uranium and Precise Measurement of 234U/238U and 235U/238U Ratios in Soil Samples Using Multi Collector Inductively Coupled Plasma Mass Spectrometry.

A new chemical separation has been developed to isolate uranium (U) using two UTEVA columns to minimize iron and thorium interferences from high background area soil samples containing minerals like monazites and ilmenite. The separation method was successfully verified in some certified reference materials (CRMs), for example, JSd-2, JLk-1, JB-1 and JB-3. The same method was applied for purification of U in Fukushima soil samples affected by the Fukushima dai-ichi nuclear power station (FDNPS) accident. Precise and accurate measurement of 234U/238U and 235U/238U isotope ratios in chemically separated U were carried out using a multi-collector inductively coupled plasma mass spectrometer (MC-ICP-MS). In this mass spectrometric method, an array of two Faraday cups (1011 Ω, 1012 Ω resistor) and a Daly detector were simultaneously employed. The precision of U isotope ratios in an in-house standard was evaluated by replicate measurement. Relative standard deviation (RSD) of 234U/238U and 235U/238U were found to be 0.094% (2σ) and 0.590% (2σ), respectively. This method has been validated using a standard reference material SRM 4350B, sediment sample. The replicate measurements of 234U/238U in SRM shows 0.7% (RSD). This developed method is suitable for separation of U and its isotope ratio measurement in environmental samples.

Impact on gadolinium anomaly in river waters in Tokyo related to the increased number of MRI devices in use.

The Gd-based contrast agents utilized in magnetic resonance imaging are difficult to remove by usual sewage treatment technology, and they enter rivers in the discharges from waste water treatment plants. Gd anomaly in rivers has been considered depends on used amount of Gd-based contrast agents. In this study, variation of Gd anomaly in rivers of Tokyo was determined by comparisons to previously reported values. The range of anthropogenic Gd was 0.1-138.8 ppt with an average value of 35.5 ppt (n = 40); in particular, the anthropogenic Gd was significantly changed depending on the location of the waste water treatment plants, and the measurement revealed significant increases in the Gd anomaly in the range of 5.0-6.6 times compared to data obtained 22 years ago. This study highlights the necessary of continuous research in setting new public policies for medical practices.

Changes of absorbed dose rate in air in metropolitan Tokyo relating to radiocesium released from the Fukushima Daiichi Nuclear Power Plant accident: Results of a five-year study.

Car-borne surveys were carried out in metropolitan Tokyo, Japan, in 2015, 2016, 2017 and 2018 to estimate the transition of absorbed dose rate in air from the Fukushima Daiichi Nuclear Power Plant accident. Additionally, the future transition of absorbed dose rates in air based on this five-year study and including previously reported measurements done in 2014 by the authors was analyzed because central Tokyo has large areas covered with asphalt and concrete. The average absorbed dose rate in air (range) in the whole area of Tokyo measured in 2018 was 59 ± 9 nGy h-1 (28-105 nGy h-1), and it was slightly decreased compared to the previously reported value measured in 2011 (61 nGy h-1; 30-200 nGy h-1). In the detailed dose rate distribution map, while areas of higher dose rates exceeding 70 nGy h-1 had been observed on the eastern and western ends of Tokyo after 2014, the dose rates in these areas have decreased yearly. Especially, the decreasing dose rate from radiocesium (Cs-134 + Cs-137) in the eastern end of Tokyo which is mainly covered by asphalt was higher than that measured in the western end which is mainly covered by forest. The percent reductions for the eastern end in the years 2014-2015, 2015-2016, 2016-2017 and 2017-2018 were 49%, 21%, 18% and 16%, and those percent reductions for western end were 26%, 18%, 6% and 3%, respectively. Additionally, the decrease for dose rate from radiocesium depended on the types of asphalt, and that on porous asphalt was larger than the decrease on standard asphalt.

IMPACT ON ABSORBED DOSE RATE IN AIR IN THE IZU ISLANDS FROM LONG HALF-LIFE RADIONUCLIDES RELEASED BY THE FUKUSHIMA DAIICHI NUCLEAR POWER PLANT ACCIDENT.

Car-borne surveys were carried out on eight islands of the Izu Islands located 339-570 km southwest of the Fukushima Daiichi Nuclear Power Plant. The mean dose rates measured in 2015, 2016 or 2017 on each island were from 12 to 47 nGy h-1, meaning that the contribution ratios of artificial radionuclides were 5-31%. Based on the environmental half-life for long half-life radionuclides (134Cs + 137Cs) measured on Izu-Oshima (3.1 y), the mean dose rates in March 2011 were estimated to be 15-53 nGy h-1 and the contribution ratios of artificial radionuclides were 11-55%. The estimated annual external effective doses were 0.06-0.21 mSv which were 13-44% of the worldwide average (0.48 mSv).