Tissue free water tritium in pine needles around a nuclear power plant

The elevation of the concentration of tissue free water tritium (TFWT) in pine needles was discernible in trees growing around a nuclear power plant. The values varied from 2.6 Bq/l to 6.1 Bq/l with a mean value of 3.8 Bq/l. Analysis of pine needles collected at Fukui City as control samples was done. The values averaged 1.7 Bq/l and fell within 1.5 B/l-1.8 Bq/l which was obtained nation-wide survey of TFWT in pine needles in Japan. The present study also revealed that reactor tritium incorporated into pine needles decreased rapidly with a half time of 6 days and then tissue free water tritium has a short retention time.     

Determination of a strong organic ligand dissolved in seawater: Thorium-complexing capacity of oceanic dissolved organic matter

Studies have been made of loose water tritium (LWT) distribution and behavior in the soil samples taken from the region within a radius of 2 km to the HWRR stack of CIAE. The analytical results show that the LWT concentrations in most soil samples of the region are in the range from 24.8 Bq/l (3.6 Bq/kg) to 116 Bq/l (16.0 Bq/kg) with an average value of 58.1±24.8 Bq/l (10.3±4.5 Bq/kg). There are two areas with a higher LWT content; the first one (4.61 · 10⁴ m²) is located near HWRR with ahighest LWT concentration of 287 Bq/l (55.8 Bq/kg) and the second one (3.27 ·10⁵ m²) is located near Lab. A with a highest LWT concentration of 2.35 · 10⁴ Bq/l (2.56 · 10³ Bq/kg). It is estimated that the LWT inventories deposited in soil of the two areas are about 1.52 · 10⁹ Bq and 1.42 · 10¹⁰ Bq, respectively. The analytical results have been evaluated by comparing the possible tritium intake of the human body with the annual limit of intake recommended by ICRP, it can be concluded that the operations of all the nuclear facilities releasing tritium in CIAE are safe without causing any notable tritium contamination.     

Development of an environmental atmospheric tritium monitoring system at the Toki site

n this study, the application for monitoring atmospheric tritium at the site of nuclear fusion facility is presented. Construction and examination of the tritium sampler and its arrangement at the site are mainly discussed. Atmospheric tritium concentrations at Toki site were determined in the sampling period from September 2000 to June 2001. Although the data for HTO were low because of their low specific activity (0.62 Bq/l), our average HT and CH₃T data were 9.1 and 3.3 mBq/m³, respectively, and systematically lower than the previously reported values at the same site, even if the considerable decay correction was carried out. Suitable monitoring points are discussed by considering the local meteorological features at the Toki site. Since the wind conditions at this site were governed by diurnal and nocturnal wind blowing to the contrary directions, it is concluded that the monitoring points should be placed at the site boundary of downwind direction of these winds. Considering that the expected levels of effluent tritium in the D-D experiment at the National Institute for Fusion Science are competitive with those in the environment, the detailed variations of the environmental tritium should be comprehended to detect minute amounts of the artificial tritium.     

Study of gas generation in real L/ILW containers

To obtain reliable estimates of the quantities and rates of the gas production in L/ILW a series of measurements was carried in the last 7 years in Hungary. The typical gas production rates were 0.05–0.2 STP litre gas/day for CO₂ and CH₄ generation, and less for H₂. No explosive gas mixture was indicated in the L/ILW drums during the investigated storage period. Compositions of headspace gases in closed L/ILW vaults were in agreement with gas generation processes observed in L/ILW drums. The stable carbon isotope measurements show that the main source of the CO₂ gas is the degradation of organic matter and indicates microbial degradation processes as the main sources of CH₄. Typical tritium activity concentrations were <10 Bq/l gas in the drums and <1,000 Bq/l gas in the vaults. Typical ¹⁴C activity values of the headspace gases were <2.0 Bq/l gas in the drums and <1,000 Bq/l gas in the vaults.     

Relation between tritium concentration and chemical composition in rain at Fukuoka

Tritium concentrations in rain collected at Fukuoka, Japan from 1982 have been measured. From May 1996 tritium concentrations and chemical species have been analyzed for each rain to examine their relationship. Recent rain was concluded not to be affected by tritium from atmospheric nuclear tests. Tritium concentrations showed a seasonal pattern, high during winter and spring and low during summer and fall and had positive correlations with non-sea-salt SO₄ ⁻², indicating a long distance transport of acidic materials as tritium from continental China.     

Tritium in a Pine Forest Ecosystem: Relation between Fresh Pine Needles, Organic Materials on a Forest Floor and Atmosphere

Tritium concentrations were analyzed in organic and water fractions of fresh pine needles, dead and degraded pine needles accumulating on a pine forest floor to examine tritium cycle in a forest ecosystem. Tritium concentration was higher in the organic fraction of dead and degraded pine needles compared to others, suggesting two tritium sources. Rain is responsible for water fractions in the samples, while atmospheric hydrogen and methane are speculated to be responsible for high tritium level in the organic fraction of dead and degraded pine needles.     

Determination of iodine-129 and iodine-127 in environmental samples collected in Japan

Analytical method for the determination of¹²⁹I and¹²⁷I in environmental samples has been developed by using radiochemical neutron activation analysis. The¹²⁹I levels in the samples such as soil (0.9–41 mBq/kg), precipitation (0.002–0.11 mBq/kg), pine needles (1.2–32 mBq/kg) and seaweed (<0.1–17 mBq/kg) collected near the nuclear facilities in Tokaimura were higher than those from the other areas in Japan. The highest¹²⁹I concentration was found in surface soil (0–5 cm), and the highest¹²⁹I/¹²⁷I ratios were found in pine needles and precipitation. The¹²⁹I/¹²⁷I ratio was higher in rice paddy soil than those in wheat field soil collected around Tokaimura, while the concentration of¹²⁹I somewhat higher in wheat field soil.     

Experimental investigation on tritium gettering with hydrogen uranyl phosphate (HUP)

At room-temperature and atmospheric pressure, using electrode disks of various sizes, under the action 4 7Vdc eletric field, we gettered tritium gas from 2.2L of air containing (0.15 18.61)×10⁸ Bq of tritium and (3000 12000) ppm of moisture during 50 hours or so the efficiency of gettering tritium was over 95%. Applying liquid scintillation counting method, we measured the tritium in the disks after gettering, and found that the amounts of tritium in the disks were equal to those reduced in the tested tritiated air.     

Evaluation of environmental tritium level in preoperational period of Cernavoda CANDU Nuclear Power Plant

In Romaia, CANDU Nuclear Power Plant with five reactors of 600 MWe is under construction at Cernavoda town and in 1996 the first reactor was put in operation. The background level of tritium concentration was determined in preoperational stage. The mean values determined are: (7.4±5.5) Bq/l in air humidity, 3.1±1.0) Bq/l in water, (3.5±0.7) Bq/l in tissue water from vegetable and (4.9±1.7) Bq/l in tissue water from cereals. The transfer parameters for deposition from atmosphere on forage and crops (P₁₄), and the contamination of land and vegetation by spray irrigation water, (P₂₄) were evaluated at (29–49) and (0.90±0.27), respectively.     

Detection of tritium and alpha decaying radionuclides in L/ILW by measurements of helium isotopes

As decay products, helium isotopes can clearly indicate the presence of tritium and alpha decaying isotopes in a closed system. This study presents the helium and neon measurements and their interpretation of long-term headspace gas investigations in L/ILW waste drums from Paks Nuclear Power Plant and closed vaults of the Radioactive Waste Treatment and Disposal Facility, Püspökszilágy, Hungary. Development of special sampling methods and preparation lines as well as isotope-analytical measurements of the headspace gas samples were done in the Hertelendi Laboratory of Environmental Studies in the ATOMKI. In the gas samples helium isotopes as well as neon isotopes have been determined mass spectrometrically. While neon content can be of atmospheric origin only, helium can be produced either by alpha decay (⁴He) or decay of tritium (³He). ³H/⁴He and He/Ne ratios have been used to determine the different origin of the helium isotopes. Helium isotope ratios always represented ³He enrichment in the headspace gases produced by the decay of the tritium in the waste. Using the recent ³He concentration in headspace gas the total amount of ³H restored in L/ILW vaults was estimated. The investigated seven different vaults were closed between 1979 and 1995 when they had been full with L/ILW. The calculated tritium activities based on the He measurements showed good agreement with the documented isotope inventory of the vaults. Typical tritium activity concentrations were between 0.1 and 10 Bq/L gas in the drums and between 10 and 1000 Bq/L gas in the vaults. Additionally, one drum showed a higher He/Ne ratio compared to air, which clearly indicates ⁴He excess, thus the presence an alpha source in the waste.     

Determination of low level85Kr and133Xe concentrations in the environment

This study was performed under the joint TRMC/INER program for the determination of low level⁸⁵Kr and¹³³Xe concentrations in the environmental air samples. Based on cryogenic adsorption of krypton and xenon on charcoal followed by chromatographic separation from other gases, the⁸⁵Kr and¹³³Xe recovered from 200 liters of atmospheric air can be determined by either on-line gas flow proportional counter or liquid scintillation counting. The recovery yields of krypton and xenon examined by using⁸⁵Kr and¹³³Xe tracers were nearly 100%. The minimum detectable activity of⁸⁵Kr and¹³³Xe by gas flow proportional counting is about 7.40 Bq. The method is satisfactory for environmental monitoring applications under abnormal conditions of nuclear facilities. However, for lower level environmental⁸⁵Kr and¹³³Xe measurements, the liquid scintillation counting method can be applied due to their extremely low detection limits (i.e. 0.107 Bq and 0.093 Bq for⁸⁵Kr and¹³³Xe, respectively). Using this method, the measurable limits of concentrations are 0.535 Bq/m³ and 0.466 Bq/m³ for⁸⁵Kr and¹³³Xe, respectively.     

Radon and tritium measurements in drinking water in a region of central Italy (Umbria)

Summary In the last years the interest in drinking and mineral water radioactivity has grown. Recently national and EU regulations replaced the previous drinking water norms with the aim to strengthen consumers security concerning drinking water quality. Perugia and Urbino Universities carried out a joint study on the radiological characterization of the water destined for human consumption in the Umbria region. The aim of this work was to produce a map of the radon and tritium concentrations in the water of this area as a basis for the implementation of hydrogeological knowledge and to determine a possible related radiological risk for the local population.²²²Rn measurements were performed by liquid scintillation and gamma-spectrometry and³H measurements by liquid scintillation. Up to now, the²²²Rn concentrations ranged 5.9-65.79 Bq/l and³H concentrations are always lower than the detection limit (8.6 Bq/l).     

Levels of artificial radionuclides and uranium in rain water collected from Ibaraki (Japan) following the Tomsk-7 accident in Russia

Measurements of some selected radionuclides were carried out in rain waters collected from Ibaraki Prefecture, Japan, following the nuclear accident at Tomsk-7, Russian Federation, in April 1993. The concentrations obtained for artificial radionuclides were⁹⁰Sr1.8 mBq l^–1,¹³⁷Cs0.1 Bq l^–1,¹³¹I0.1 Bq l^–1 and¹²⁹I4 Bq l^–1. Uranium (²³⁸U) concentrations in rainfalls in April 1993 were 6.3–39 ng l^–1. These data were compared to control values obtained previously and there was no appreciable influence on the radioactivity levels in Japan after the Tomsk-7 accident. Since only limited data on the concentrations of¹²⁹I and uranium in rain water are available, these new analytical results contribute to understanding the background levels for these nuclides.     

Environmental monitoring as an important tool for safeguards of nuclear material and nuclear forensics

Summary The use of environmental monitoring as a technique to identify activities related to the nuclear fuel cycle has been proposed by international safeguards organizations. The elements specific for each kind of nuclear activity, or “nuclear signatures”, inserted in the ecosystem can be intercepted by different live organisms. This work demonstrates the technical viability of using pine needles as bioindicators of nuclear signatures associated with uranium enrichment activities. Additionally, it proposes the use of HR-ICP-MS to identify the signature corresponding to that kind of activities in the ecosystem. Nitric acid solutions, used to wash pine needles sampled near nuclear facilities and containing only 0.1 mg ^. kg^-1 of uranium, exhibit a n(²³⁵U)/n(²³⁸U) isotopic abundance ratio of 0.0092±0.0002, while solutions originated from samples collected at places located more than 200 km far from activities related to the nuclear fuel cycle exhibit a value of 0.0074±0.0002. Similar results were obtained for sample solutions prepared using the acid leaching process. The different values of n(²³⁵U)/n(²³⁸U) isotopic abundance ratio obtained permit to confirm the presence of anthropogenic uranium and demonstrate the viability of using the methodology proposed in this work.     

Efficiency of tritium enrichment by electrolytic cell with multi-nickel-plates electrode and its application to the determination of tritium in environmental water

For the purpose of speeding up the tritium enrichment by electrolysis, we have produced an electrolytic cell with the multi-plate-electrode system instead of the commonly used single-plate-electrode, and examined the efficiencies for the tritium enrichment under the conditions of different current densities and electrode gaps. From the results, the tritium recovery and the separation factor beta were found to be maximized under the condition of 70 mA/cm2 of current density and 1.6 mm of electrode gap, and they were 90 percent and 23, respectively. Using this cell, it took 28 hours to reduce 100 ml of a sample water to 10 ml, and took 2 days, including the time required for other operations, to determine the tritium concentration of 1.85 Bq/l (50 pCi/l) with the counting error of within +/- 10 percent. This method has been applied to determining the tritium concentrations of environmental samples from Yamato River region during July 1981-February 1983. They were in the range of 1.11-9.48 Bq/l (30-256 pCi/l).     

A recent drilling program to investigate radionuclide migration at the Nevada Test Site

Recent drilling affords new opportunities to investigate the occurrence, distribution, and transport of radionuclides above and below the water table at the Nevada Test Site (NTS), Nye County, Nevada. This program is unique because of elevated levels of radioactivity encountered during drilling (>3.7E+6Bq/l³H), extreme completion depths (>950 m), and the expense of constructing new wells (>$1E+6/borehole). Sites of five nuclear tests have been drilled. Three of the events were fired in Yucca Flat which is a hydrologically closed basin and two were fired in fractured volcanics of Pahute Mesa. Results from Yucca Flat indicate that volatile and refractory radionuclides fractionated at zero time, are not highly mobile under saturated conditions. In contrast, boreholes completed on Pahute Mesa intercept high concentrations of tritium (>3.7E+6Bq/l³H) and other radionuclides transported more than 300 m from event cavities as dissolved species or as colloids.     

An improved apparatus for the determination of krypton-85 and xenon-133 in an emergency situation

A simple and portable apparatus was developed for measurements of⁸⁵Kr and¹³³Xe that would be released into the atmosphere in an emergency situation of nuclear facilities. The method is based on cryogenic adsorption of these gases on charcoal followed by chromatographic separation from other gases. The⁸⁵Kr and¹³³Xe recovered from atmospheric air are determined separately by liquid scintillation counting. It takes about 1 hour for the stepwise determination of⁸⁵Kr and¹³³Xe. The atmospheric concentration of 3·10^–3 Ci per m³ air (1.1·10² Bq/m³ air) is measurable for both nuclides with 20% counting error.     

Monitoring of atmospheric 3H around Narora Atomic Power Station

Atmospheric tritium activity is measured regularly around Narora Atomic Power Station (NAPS) since gaseous waste, which contains tritium, is being released through a 145 m high stack at NAPS site. Atmospheric data collected during 2004–2008 shows a large variation of ³H concentration in air, fluctuating in the range of ≤0.2–91.6 Bq m^?3. Significantly, higher tritium levels were measured in samples near the site boundary (1.6 km) of NAPS compared to off-site locations. The atmospheric dilution factor was found to be in the range of 1.1 × 10^?7–7.3 × 10^?7 s m^?3. The scavenging ratio of NAPS site was found to be varying from 0.2 × 10⁴ to 14.1 × 10⁴ (Bq m^?3 rain water per Bq m^?3 air). The inhalation dose to a member of general public at different distances (1.6–30 km) from NAPS site was found to be ranged from 0.08–0.21 μSv year^?1.     

Tritium activity levels in drinking water of Adana,Turkey

Tritium activity in potable drinking water samples from Adana city were measured using liquid scintillation counting after distillation procedure. The results exposed that the activity concentrations of the tritium measured in one-third of these samples were lower than minimum detectable activity which has a value of 2 Bq/L for counting time of 1,500 min. However, the maximum and mean value of the tritium activity was found to be 9.1 Bq/L (77.3 TU) and 7.0 Bq/l (59.4 TU), respectively. These values were substantially below the 100 Bq/L which is normative limit in Turkey for waters intended for human consumption. The highest values of annual effective dose received by infants, children and adults due to measured tritium activity were estimated as 0.041, 0.057 and 0.120 μSv/y, respectively.     

Reproducible tritium generation in electrochemical cells employing palladium cathodes with high deuterium loading

Reproducible tritium generation well above background has been observed in tightly closed D₂SO₄-containing cells in four out of four Pd wire cathodes of one type. Tritium analysis was performed before and after each experiment on the Pd, the electrolyte and the gas in the head space. No tritium generation was observed in four identical Pd cathodes in H₂SO₄ cells operated at the same time under the same conditions. A cyclic loading-unloading regime with low current densities, rather than the usual continuous constant current regime, was employed to attain D/Pd and H/Pd loadings of 1±0.05 reproducibly. D/Pd loadings greater than 0.8±0.05 appear to be necessary to generate tritium. The largest amount of tritium, generated in 7 days of continuous electrolysis, was 2.1 × 10¹¹ tritium atoms, compared with a background of 4 × 10⁹ tritium atoms. The concentration of tritium and its axial distribution in the Pd were determined and concentrations of up to 9 × 10¹⁰ atoms/g Pd were found compared with a maximum background of 5 × 10⁸ atoms g⁻¹. The T/D ratio in the Pd is about 100 times larger than in the electrolyte or gas and indicates that tritium generation occurs in the Pd interior rather than at its surface. No tritium generation was observed in two other types of Pd electrodes in D₂SO₄, despite the attainment of D/Pd ratios near 1:1. Thus high D/Pd ratios appear to be a necessary but not sufficient condition for tritium generation in D₂SO₄ electrolysis.