Improvement of spectral analysis using a NaI(Tl) scintillation spectrometer to evaluate ambient gamma dose rates from primordial radionuclides.

In-situ measurements by gamma-ray spectrometry using a NaI(Tl) scintillation spectrometer are performed to discriminate primordial and artificial radionuclides contributing to ambient gamma dose rates in the living environment to quantify prolonged influence of nuclear accidents. However, low energy resolution of the spectrometer causes poor discrimination in the measurements at high-dose-rate points, which leads to overestimation of ambient gamma dose rate from the primordial radionuclides. The present study clarified that photon fluxes originating from 40K and 214Bi were affected by the presence of 134Cs, whereas those from 208Tl were independent of it. In addition, the absorbed dose rates in air were strongly correlated with the 208Tl photon fluxes. These findings indicate that 208Tl photon fluxes can be used to evaluate absorbed dose rates in air from the primordial radionuclides. When estimated from the 208Tl photon fluxes only, the absorbed dose rates in air in Namie Town and Okuma Town, locations affected by the Fukushima Dai-ichi Nuclear Power Plant accident, were 19-71 and 20-47 nGy h-1, respectively.

Distribution of strontium-90 in soils affected by Fukushima dai-ichi nuclear power station accident in the context of cesium-137 contamination.

90Sr and 137Cs activity concentrations were determined by radiometric methods in 76 soil samples (soil, litter, rain gutter deposit, and roadside sediment samples) affected by the Fukushima Dai-ichi Nuclear Power Station (FDNPS) accident and collected from the Fukushima exclusion zone. The 90Sr and 137Cs activity concentrations were in the range of 3 to 1050 Bq kg-1 (median 82 Bq·kg-1) and 0.7 to 6770 kBq·kg-1 (median 890 kBq·kg-1), respectively (decay correction date: March 15, 2011). A strong positive correlation was found between 90Sr and 137Cs activity concentration and higher mobility of 90Sr was confirmed in Japanese soil samples. The activity ratio of 90Sr/137Cs in 85% of all samples was in the range of 5.0 × 10-5 to 5.0 × 10-4 with a median of 1.2 × 10-4. From the activity ratio values it was concluded that the 90Sr released to the atmosphere was only around 0.0003-0.02 PBq which is negligible compared to the Chernobyl accident (∼10 PBq) or other nuclear accident contaminations. From the standpoints of radioecology and radiation safety, 137Cs remains the primary pollutant of the FDNPS accident.

Effect of operating variables on the separation of radiostrontium from aqueous matrices with ion-selective solid-phase extraction systems.

Radiostrontium (r-Sr: 90Sr) is one of the primary fission products in nuclear power plants and generates liquid radioactive waste when intermixed to the aqueous matrix. Therefore, separation or preconcentration of r-Sr from the aqueous matrices is necessary for environmental monitoring or nuclear forensics. The solid-phase extraction (SPE) approach is prevalently used for r-Sr isolation and to design matrix-specific methods, while generalized SPE-assisted operating protocols are not proposed by far. In the current work, four different SPEs, namely AnaLig Sr-01, Eichrom Sr, Triskem TK100, and Eichrom DGA, were evaluated for selective separation of Sr from aqueous matrices. Operating variables, e.g., solution acidity, washing solvent, eluent-type or volume, loading or elution flow-rate, were varied to optimize the SPEs performance. The objective was to ascertain the operating variables for maximum Sr-separation yield from aqueous environmental samples with the SPEs mentioned above. In addition, the Sr-separation efficiency of SPEs was evaluated by calculating the separation factor (SFSr/M) between Sr and interfering elements to r-Sr (M = Ca, Mg, Ba, or Y), and the Sr-retention capacity of the SPEs was determined. Finally, the optimized operating variables for the evaluated SPEs were used to construct protocols for r-Sr separation from aqueous matrices. Real 90Sr contaminated aqueous samples from the Chernobyl nuclear power plant cooling pond were treated by those protocols, and the results are validated comparing with the IAEA-recommended classical protocol. All the SPEs were able to isolate Sr at varying extents from matrices at the optimum conditions, even at much higher contents of interfering elements. Eichrom Sr or AnaLig Sr-01 showed better Sr-retention capability among the SPEs, while Triskem TK100 showed superiority over other SPEs regarding Sr-selectivity.

Effects of Storage Time and Pre-Etching Treatment of CR-39 Detectors on Their Response to Alpha Radiation Exposure.

Radon passive monitors based on solid state nuclear track detectors (SSNTD), especially CR-39, are widely used in radon and thoron studies. They may be subjected to the influence of external factors, like changing of temperature, humidity, and pressure, both before and during the measurement. Evaluation of the exposed detectors involves chemical processing, whose conditions also influence the measurement results. The aim of this study was to check several factors, as to whether they may modify the response of CR-39 detector: concerning the phase before evaluation, storage time, and temperature during storage; and concerning the evaluation procedure, etching time, and pre-etching treatment using hot water and carbon dioxide atmosphere. Two experiments were conducted by irradiation of CR-39 detectors using alpha particles emitted from a mono-energetic 241Am source and exposed in radon atmosphere. Track density dependence of the age of production was found to be statistically not significant. On the other hand, pre-etching treatment using hot water and carbon dioxide with different etching times showed statistically significant effects on track area, track sensitivity, and roundness. It was concluded that there are simple methods to increase performance of nuclear track detectors, and that storage time is not a factor of concern.

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.

Accurate and precise determination of 90Sr at femtogram level in IAEA proficiency test using Thermal Ionization Mass Spectrometry.

A novel method for the determination of ultra-trace level 90Sr has been recently developed applying thermal ionization mass spectrometry (TIMS). The method includes the chemical separation of Zr (isobaric interference of 90Zr) from the samples followed by determination of 90Sr/88Sr abundance  sensitivity (2.1 × 10-10). The analytical performance of this method was assessed in the IAEA-TEL 2017-3 worldwide open proficiency test. For 90Sr determination, tap water and milk powder samples were distributed amongst the participant laboratories with reference values of 11.2 ± 0.3 Bq kg-1 (2.2 ± 0.1 fg g-1) and 99.9 ± 5.0 Bq kg-1 (19.5 ± 1.0 fg g-1), respectively. The stable Sr concentrations were 39.4 ± 0.9 ng g-1 and 2.5 ± 0.1 µg g-1 while the 90Sr/88Sr isotope ratios were 6.47 ± 0.17 × 10-8 and 9.04 ± 0.45 × 10-9 in the tap water and milk powder samples, respectively. For TIMS measurement, 50 mL water and 1 g milk powder samples were taken for analysis. This TIMS method demonstrated an impressive accuracy (relative bias of 4.2% and -2.1%, respectively) and precision (relative combined uncertainty of 4.1% and 7.6%, respectively) when compared with radiometric techniques. For the first time in the history of inorganic mass-spectrometry, 90Sr analysis using a TIMS instrument is confirmed by an independent proficiency test.

OCCUPATIONAL EXPOSURE ASSESSMENT AT A THERAPEUTIC RADON SPA FACILITY IN HUNGARY.

In order to estimate occupational exposure of workers in a therapeutic radon spa facility, radon concentration in the workplace air was investigated at Markhot Ferenc Hospital, Eger, Hungary. The investigated balneotherapeutic facility and its natural hot spa water are used for treatments and rehabilitations of rheumatic patients. Radon concentration, radon decay products at a bathhouse, treatment rooms and a consultation room were continuously measured in August and September 2018. In the present study, different levels of radon concentration among the observation sites and its clear temporal variations were found, though radon concentrations in the investigated sites were below 300 Bq m-3. Regarding such radon fluctuation and low equilibrium factor level (0.1), the annual effective doses of workers are estimated to be around 0.5 mSv year-1.

EFFECTIVE DOSES ESTIMATED FROM THE RESULTS OF DIRECT RADON AND THORON PROGENY SENSORS (DRPS/DTPS), EXPOSED IN SELECTED REGIONS OF BALKANS.

The main contribution to population exposure is due to radon and thoron progenies and not radon itself. The aim of this study was therefore to estimate annual effective dose using the results of Direct Radon and Thoron Progeny Sensors were exposed in 69 selected schools and 319 dwellings in several regions of Balkans: in Serbia: regions of Sokobanja and Kosovo and Metohija, Republic of Macedonia, Republic of Srpska and Slovenia. Obtained average total effective doses are in the range from 0.22 mSv a-1 (schools in Republic of Srpska) to 2.5 mSv a-1 (dwellings in Kosovo) and are below the reference level of 10 mSv a-1 recommended by International Commission on Radiological Protection.

Method for 90Sr Analysis in Environmental Samples Using Thermal Ionization Mass Spectrometry with Daly Ion-Counting System.

In this work, a new 90Sr analysis method was developed using the Isotopx Ltd., Phoenix X62 thermal ionization mass spectrometer (TIMS). Excellent ion beam sensitivity was demonstrated with the detection of 1 mBq (0.2 fg) 90Sr on a Daly ion-counting system. The abundance sensitivity for the 90Sr/88Sr ratio was 2.1 × 10-10, and this could ensure measurement of 100 Bq·kg-1 (19 fg·g-1) 90Sr in an environmental sample with 100 µg·g-1 stable strontium concentration. For analytical method validation, 90Sr was determined in two certified reference materials, for example, wild berry (IRMM-426) and freshwater lake sediment (NIST-4354), for the first time in the history of TIMS. This mass spectrometry method is faster than conventional radiometric techniques; however, interference from 90Zr and peak tailing on the higher mass side from 88Sr must be considered for a reliable 90Sr determination.

Strontium-90 activity concentration in soil samples from the exclusion zone of the Fukushima daiichi nuclear power plant.

The radioactive fission product (90)Sr has a long biological half-life (˜18 y) in the human body. Due to its chemical similarity to calcium it accumulates in bones and irradiates the bone marrow, causing its high radio-toxicity. Assessing (90)Sr is therefore extremely important in case of a nuclear disaster. In this work 16 soil samples were collected from the exclusion zone (<30 km) of the earthquake-damaged Fukushima Daiichi nuclear power plant, to measure (90)Sr activity concentration using liquid scintillation counting. (137)Cs activity concentration was also measured with gamma-spectroscopy in order to investigate correlation with (90)Sr. The (90)Sr activity concentrations ranged from 3.0 ± 0.3 to 23.3 ± 1.5 Bq kg(-1) while the (137)Cs from 0.7 ± 0.1 to 110.8 ± 0.3 kBq kg(-1). The fact that radioactive contamination originated from the Fukushima nuclear accident was obvious due to the presence of (134)Cs. However, (90)Sr contamination was not confirmed in all samples although detectable amounts of (90)Sr can be expected in Japanese soils, as a background, stemming from global fallout due to the atmospheric nuclear weapon tests. Correlation analysis between (90)Sr and (137)Cs activity concentrations provides a potentially powerful tool to discriminate background (90)Sr level from its Fukushima contribution.

Optimization of the Timepix chip to measurement of radon, thoron and their progenies.

Radon and thoron as well as their short-lived progenies are decay products of the radium and thorium series decays. They are the most important radionuclide elements with respect to public exposure. To utilize the semiconductor pixel radiation Timepix chip for the measurement of active and real-time alpha particles from radon, thoron and their progenies, it is necessary to check the registration and visualization of the chip. An energy check for radon, thoron and their progenies, as well as for (241)Am and(210)Po sources, was performed using the radon and thoron chambers at NIRS (National Institute of Radiological Sciences). The check found an energy resolution of 200 keV with a 14% efficiency as well as a linear dependency between the channel number (cluster volume) and the energy. The coefficient of determination r(2) of 0.99 for the range of 5 to 9 MeV was calculated. In addition, an offset for specific Timepix configurations between pre-calibration for low energy from 6 to 60 keV, and the actual calibration for alpha particles with energies from 4000 to 9000 keV, was detected.

Invited article: in situ comparison of passive radon-thoron discriminative monitors at subsurface workplaces in Hungary.

During a one-year long measurement period, radon and thoron data obtained by two different passive radon-thoron discriminative monitors were compared at subsurface workplaces in Hungary, such as mines (bauxite and manganese ore) and caves (medical and touristic). These workplaces have special environmental conditions, such as, stable and high relative humidity (100%), relatively stable temperature (12°C-21°C), low or high wind speed (max. 2.4 m s(-1)) and low or elevated aerosol concentration (130-60,000 particles m(-3)). The measured radon and thoron concentrations fluctuated in a wide range among the different workplaces. The respective annual average radon concentrations and their standard deviations (in brackets) measured by the passive radon-thoron discriminative monitor with cellulose filter (CF) and the passive radon-thoron discriminative monitor with sponge filter (SF) were: 350(321) Bq m(-3) and 550(497) Bq m(-3) in the bauxite mine; 887(604) Bq m(-3) and 1258(788) Bq m(-3) in the manganese ore mine; 2510(2341) Bq m(-3) and 3403(3075) Bq m(-3) in the medical cave (Hospital Cave of Tapolca); and 6239(2057) Bq m(-3) and 8512(1955) Bq m(-3) in the touristic cave (Lake Cave of Tapolca). The respective average thoron concentrations and their standard deviation (in brackets) measured by CF and SF monitors were: 154(210) Bq m(-3) and 161(148) Bq m(-3) in the bauxite mine; 187(191) Bq m(-3) and 117(147) Bq m(-3) in the manganese-ore mine; 360(524) Bq m(-3) and 371(789) Bq m(-3) in the medical cave (Hospital Cave of Tapolca); and 1420(1184) Bq m(-3) and 1462(3655) Bq m(-3) in the touristic cave (Lake Cave of Tapolca). Under these circumstances, comparison of the radon data for the SF and CF monitors showed the former were consistently 51% higher in the bauxite mine, 38% higher in the manganese ore mine, and 34% higher in the caves. Consequently, correction is required on previously obtained radon data acquired by CF monitors at subsurface workplaces to gain comparable data for SF monitors. In the case of thoron, the data were unreliable and no significant tendency was seen during the comparison therefore comparison of previously obtained thoron data acquired by either CF or SF is doubtful. There was probable influence by relative humidity on the detection response; however, the effects of the high wind speed and elevated aerosol concentration could not be excluded. The results of this study call attention to the importance of calibration under extreme environmental conditions and the need for using reliable radon-thoron monitors for subsurface workplaces.

Dose estimation and radon action level problems due to nanosize radon progeny aerosols in underground manganese ore mine.

One of the essential parameters influencing of the dose conversion factor is the ratio of unattached short-lived radon progeny. This may differ from the value identified for indoor conditions when considering special workplaces such as mines. Inevitably, application of the dose conversion factors used in surface workplaces considerably reduces the reliability of dose estimation in the case of mines. This paper surveyed the concentration of radon and its short-lived radon progeny and identified the unattached fraction of short-lived radon progeny. As well equilibrium factor during the month of August was calculated simultaneously at two extraction faces in a manganese ore mine. During working hours the average radon concentrations were 220 Bq m(-3) and 530 Bq m(-3) at Faces 1 and 2; the average short-lived progeny concentration was 90 Bq m(-3) and 190 Bq m(-3), the average equilibrium factors were 0.46 and 0.36, and the average unattached fractions were 0.21 and 0.17, respectively. The calculated dose conversion factor was between 9 and 27 mSv WLM(-1), but higher values could also be possible.

Effect of radon measurement methods on dose estimation.

Different radon measurement methods were applied in the old and new buildings of the Turkish bath of Eger, Hungary, in order to elaborate a radon measurement protocol. Besides, measurements were also made concerning the radon and thoron short-lived decay products, gamma dose from external sources and water radon. The most accurate results for dose estimation were provided by the application of personal radon meters. Estimated annual effective doses from radon and its short-lived decay products in the old and new buildings, using 0.2 and 0.1 measured equilibrium factors, were 0.83 and 0.17 mSv, respectively. The effective dose from thoron short-lived decay products was only 5 % of these values. The respective external gamma radiation effective doses were 0.19 and 0.12 mSv y(-1). Effective dose from the consumption of tap water containing radon was 0.05 mSv y(-1), while in the case of spring water, it was 0.14 mSv y(-1).

Comparison of urinary excretion of radon from the human body before and after radon bath therapy.

Theoretically, the human body absorbs radon through the lungs and the skin and excretes it through the lungs and the excretory organs during radon bath therapy. To check this theory, the radon concentrations in urine samples were compared before and after radon bath therapy. During the therapy, the geometric mean (GM) and the geometric standard deviation of the radon concentration in air and in the bath water were 979 Bq m(-3), 1.58 and 73.6 Bq dm(-3), 1.1, respectively. Since radon was detected in each urine sample (GM around 3.0 Bq dm(-3)), urinary excretion of radon was confirmed. The results of this study can neither reject nor confirm the hypothesis of radon absorption through the skin. A 15 times higher increment of inhaled radon level did not cause significant changes in radon of urine samples.

International intercomparisons of integrating radon detectors in the NIRS radon chamber.

An international intercomparison of integrating detectors was conducted at NIRS (National Institute of Radiological Science, Japan) with a 24.4 m(3) inner volume walk-in radon chamber that has systems to control radon concentration, temperature and humidity. During the first intercomparison (05.2007) four groups participated from four countries and for the second intercomparison (10.2007) 17 participants were involved from 11 countries. Most of detectors are in good agreement with each other when compared to the radon level provided by the radon chamber. It appeared that the 70% of detectors are unified within the 20% margin of uncertainty.

Study on endocronological effects of radon speleotherapy on respiratory diseases.

BACKGROUND: Radon, as a radioactive noble gas of natural origin, is generally present in the atmosphere of caves during the speleotherapeutic treatment of different diseases. However, the role of radon in the therapeutic effect is not fully clarified yet. Endocrine parameter levels may be influenced by radon-like endocrine levels in balneotherapeutic treatments (bath treatment). For this reason changes of these parameters were examined in this study. PATIENTS AND METHOD: A total of 81 speleotherapy patients were involved in the survey. They spent four hours daily in Tapolca Cave, five days a week, for two weeks. In this study, the thyreoiedea stimulating hormone, free triiodine-tironin, free thyroxine, prolactine, cortisol, dehydroepiandrosterone sulphate, adrenocorticotropic hormone, and beta endorphine levels of the body were examined before and after the treatment. RESULTS: After statistical analysis of the data a significant decrease of cortisol levels of patients was found, which was not directly correlated with radon concentration. In the case of thyroid hormones, there were no significantly detectable changes of the hormone levels except for low radon concentration levels a significant decrease in the free thyroxine and the thyreoiedea stimulating hormone level of male patients was observed. CONCLUSION: Speleotherapy has an effect on the level of endocrine hormones; however, no direct correlation with differences in radon level was found. For patients whose endocrine levels fell outside the normal endocrine parameter values, more striking changes in endocrine hormone levels were seen, but changes of these parameters could not be statistically analyzed due to the small number of cases.

Does balneotherapy with low radon concentration in water influence the endocrine system? A controlled non-randomized pilot study.

Radon bath is a well-established modality of balneotherapy for the management of degenerative musculoskeletal disorders. The present study was conducted to ascertain whether baths of relatively low (80 Bq/l) radon concentration have any influence on the functioning of the endocrine system. In the study, a non-randomized pilot study, 27 patients with degenerative musculoskeletal disorders received 30-min radon baths (of 31-32 degrees C temperature and 80 Bq/l average radon concentration) daily, for 15 days. Twenty-five patients with matching pathologies were subjected to balneotherapy according to the same protocol, using thermal water with negligible radon content (6 Bq/l). Serum thyroid stimulating hormone, prolactin, cortisol, adrenocorticotropic hormone, and dehydroepiandrosterone levels were measured before and after a balneotherapy course of 15 sessions. Comparison of the accumulated data using the Wilcoxon test did not reveal any significant difference between pre- and post-treatment values or between the two patient groups. It is noted that while the beneficial effects of balneotherapy with radon-containing water on degenerative disorders is widely known, only few data have been published in the literature on its effect on endocrine functions. The present study failed to demonstrate any substantial effect of thermal water with relatively low radon content on the functioning of the endocrine system.