Rain scavenging of tritiated water vapour: a numerical Eulerian stationary model

The tradition in tritium washout modeling is to unite the washout model with a Gaussian plume model describing dispersion of tritium vapour in the atmosphere. In the present study, an alternative approach is proposed. A numerical Eulerian model that describes washout independently of dispersion is developed.The sensitivity analysis to model parameters has shown that the washout process is influenced most significantly by rainfall parameters and air temperature: different raindrop size distributions cause differences of up to about 70% in the washout outputs; a change of 15 °C in the air temperature causes an effect of about 50%.Results are presented showing calculated values of washout outputs (tritium concentration in rain, tritium downward flux, washout coefficient) for different tritium vapour profiles, rainfall rates and air temperatures. The general conclusion is that the washout process is too complex to be described comprehensively by the simple washout coefficient concept. We suggest the approach proposed here for directly calculating the tritium downward flux and concentration in the rainwater is preferable.     

Observed half-lives of 3H, 90Sr and 137Cs in hydrosphere in the Vltava River basin (Bohemia)

A near field study was set up to follow the effects of the Temelin nuclear power plant construction. Reference levels of artificial radionuclides were monitored in the Vltava River upper course and its tributaries in the period 1990-2001. Monitoring continued even after the waste water release startup during the pilot operation in 2002. The assessment of the (90)Sr and (137)Cs concentrations histories in ground water, river bottom sediments and fish showed a decreasing trend. This trend was not influenced by the nuclear power plant pilot operation. In the case of tritium, trend of increasing concentration had been already observed since the pilot operation startup. The monitoring of changes in concentrations of artificial and natural radionuclides in influenced and uninfluenced profiles will be maintained to assess the possible influence of the operation of the Temelin nuclear power plant.     

Study of the comparative dynamics of the incorporation of tissue free-water tritium (TFWT) in bulrushes (Typha latifolia) and carp (Cyprinus carpio) in the Almaraz nuclear power plant cooling reservoir

The Almaraz nuclear power plant (Spain) uses the water of Arrocampo reservoir for cooling, and consequently raises the radioactive levels of the aquatic ecosystem of this reservoir. From July 2002 to June 2005, monthly samples of surface water, bulrushes (Typha latifolia) and carp (Cyprinus carpio) were collected from this reservoir. They were analyzed to determine the temporal evolution of the levels of ³H in surface water and of its transfer from the surface water to free-water in the tissues (TFWT) of the aforementioned two organisms. The tritium levels in the surface water oscillate with a biannual period, with their values in the study period ranging between 53 and 433 Bq/L. The incorporation of tritium to bulrushes and carp was fairly similar, the respective mean concentration factors being 0.74 and 0.8 (unitless, as Bq/L tissue water per Bq/L reservoir water). The temporal evolution of the levels fairly closely followed that observed for the surface water tritium, although detailed analysis showed the dominant periodicity for the bulrushes to be annual. This difference reflects the influence on the incorporation of tritium to bulrushes of diverse environmental and metabolic factors, especially evapotranspiration and the seasonal growth of this plant.     

The distribution of tritium in the terrestrial and aquatic environments of the Creys-Malville nuclear power plant (2002-2005)

The Creys-Malville nuclear plant, located on the left bank of the Rh?ne, was shut down in 1998. The facilities are currently in their initial stage of dismantling. In order to establish a baseline for tritium in the vicinity of the site prior to the main dismantling phase, we carried out a monitoring program between 2002 and 2005 in the main terrestrial and aquatic compartments of the local environment. Tritium levels in the groundwaters and in the Rh?ne waters correspond to the regional tritium concentration in precipitation. The data obtained for the terrestrial environment are also in good agreement with the regional background and do not show any specific signature linked to the nuclear plant. The various aquatic compartments of the Rh?ne (fish, plant, sediment) are significantly enriched in tritium both upstream and downstream of the power plant: although Tissue-Free Water Tritium concentrations are in equilibrium with the river water, the non-exchangeable fraction of organic bound tritium in plants and fishes shows values which outpace the river water background by one to two orders of magnitude, and up to four to five orders of magnitude in the sediments. This tritium anomaly is not related to the nuclear plant, as it is already present at the Swiss border 100km upstream of the site. Although fine particles of tritiated polystyrene entering the composition of the luminous paints used by the clock industry have been suspected on several occasions, the exact nature and the origin of this tritium source remain unknown and require further investigations.     

Dispersion of 222Rn from two New Zealand geothermal power plants

The dispersion of ²²²Rn from emitted waste gases at Wairakei geothermal power station, New Zealand, is modelled. It is concluded that resulting concentrations in the nearby township of Taupo will never exceed the maximum permissible in any meteorological situation. The greatest possible accumulation is calculated to be less than one eighth of the normal background radon concentration. A more realistic set of assumptions predicts long-term mean concentrations about 4% of background levels. A new geothermal power station, Ohaaki, a factor of three times more distant, is calculated to produce ten times lower concentrations than Wairakei. Measurements using a few passive solid-state radon detectors show that the natural variation of radon concentrations greatly exceeds any calculated contribution from either geothermal station; hence, much of the radon is probably due to more local minor sources. Local sources have increased due to draw-off of ground water by the Wairakei station. Thus, there could be some indirect contribution to radon concentrations by its operation. The measured six-month integrated mean radon concentration at Taupo is a significant fraction of the maximum permissible concentration. It seems likely that natural sources alone may lead to levels in air which are above the maximum when temperature inversion exists. It is concluded that these two geothermal power plants are unlikely to produce concentrations of radon hazardous to the population or to plant workers.     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

210Pb deposition in the far East Asia: controlling factors of its spatial and temporal variations

In order to better understand the behavior of ²¹⁰Pb deposition in Far East Asia, comprehensive data of monthly ²¹⁰Pb deposition, which includes several time-series and spatial distribution data at 14 stations in Japan and 2 stations in Taiwan, were analyzed. Pb-210 deposition at most of the sites exhibited a typical seasonal change with higher values in winter and lower values in summer; especially, the greatest ²¹⁰Pb deposition in the world occurred in winter at sites beside the Japan Sea. The deposition behavior of ²¹⁰Pb in Far East Asia differed between winter and summer. The meteorological phenomenon peculiar to winter of the Japan Sea side, i.e., formation of the Japan Sea convergence zone, might cause the high ²¹⁰Pb concentration in rainwater, as may heavy snowfall. The ²¹⁰Pb concentration in rainwater showed long-term variability, although this differed between winter and summer. This long-term variability may be related to climatological factors such as El Niño.     

C, δC and total C content in soils around a Brazilian PWR nuclear power plant

Nuclear power plants release ¹⁴C during routine operation mainly as airborne gaseous effluents. Because of the long half-life (5730 years) and biological importance of this radionuclide (it is incorporated in plant tissue by photosynthesis), several countries have monitoring programs in order to quantify and control these emissions. This paper compares the activity of ¹⁴C in soils taken within 1 km from a Brazilian nuclear power plant with soils taken within a reference area located 50 km away from the reactor site. Analyses of total carbon, δ¹³C and ¹³⁷Cs were also performed in order to understand the local soil dynamics. Except for one of the profiles, the isotopic composition of soil organic carbon reflected the actual forest vegetation present in both areas. The ¹³⁷Cs data show that the soils from the base of hills are probably allocthonous.     

Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

Inventories of Pu, Cs, and excess Pb in sediments from freshwater and brackish lakes in Rokkasho, Japan, adjacent to a spent nuclear fuel reprocessing plant

We investigated the vertical profiles of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_ex) in sediment core samples obtained from two freshwater lakes and two brackish lakes situated near the first commercial spent nuclear fuel reprocessing plant in Rokkasho, Japan, before the final test of the plant using actual spent nuclear fuel. The inventory of ^239+240Pu in those lakes was larger than that in soil in Rokkasho, which indicated the inflow of ^239+240Pu from the catchment area in addition to direct deposition on the lake surfaces. The ¹³⁷Cs inventory in sediments of the brackish lakes was lower than that in the soil, which showed that part of the ¹³⁷Cs was removed from the sediments by the brackish water or that it was not deposited into the sediments, because of the high solubility of Cs in brackish water. The ¹³⁷Cs inventory in sediments of the freshwater lakes was higher than that of the brackish lakes, and comparable with that in soil except for one core sample out of four. The ^239+240Pu/¹³⁷Cs ratio in freshwater lake sediments was higher than that in soil, and that indicated that part of the ¹³⁷Cs was lost from the sediments. The low inventory of ¹³⁷Cs may be attributable to competition for absorption sites in sediments with ammonium ions formed in the reducing environment which occurs from summer to fall in the sediments. Those data will be used as background data on the artificial radionuclides in the lakes to assess the effect of released radionuclides on their concentrations.     

Distribution of radionuclides in the guano sediments of Xisha Islands, South China Sea and its implication

Several natural and anthropogenic radionuclides (²¹⁰Pb, ²²⁶Ra and ¹³⁷Cs) in guano-phosphatic coral sediments and pure guano particles collected from Ganquan, Guangjin, Jinqing and Jinyin Islands of the Xisha archipelago, South China Sea, were analyzed. The Constant Initial Concentration (CIC) model and the Constant Rate of Supply (CRS) model were applied for age calculation. The average supply rate of ²¹⁰Pb was 126 Bq m⁻² a⁻¹, very close to the flux of northern hemisphere average (125 Bq m⁻² a⁻¹). The activities of anthropogenic radionuclides in the sediments were very low, indicating that human nuclear tests did not notably impact this region. The main source of radionuclides in the sediments was from atmospheric precipitation, and the organic matter derived from plant and produced by nutrient-rich guano could further enhance them.     

Monitoring and assessment of radionuclide discharges from Temelín Nuclear Power Plant into the Vltava River (Czech Republic)

The paper summarizes impacts of the Temelín Nuclear Power Plant (NPP) on the Vltava and Labe River basins. The study is based on the results of long-term monitoring carried out before the plant operation (1989–2000), and subsequently during the plant operation (2001–2005). In the first period, the main objective was to determine background radionuclide levels remaining in the environment after global fallout and due to the Chernobyl accident. A decrease in the concentrations of ⁹⁰Sr, ¹³⁴Cs and ¹³⁷Cs, which was observed before the plant operation, continued also during the subsequent period. Apart from tritium, the results of the observation did not indicate any impacts of the plant on the concentrations of activation and fission products in the hydrosphere. The annual average tritium concentrations in the Vltava River were in agreement with predicted values. The maximum annual average tritium concentration (13.5 Bq L⁻¹) was observed in 2004 downstream from the wastewater discharge in the Vltava River at Solenice. Estimated radiation doses for adults due to intakes of river water as drinking water contaminated by tritium are below 0.1 μSv y⁻¹.     

A follow up of the decrease of non exchangeable organically bound tritium levels in the surroundings of a nuclear research center

In the past decades limited amounts of tritium were handled on the CEA site of Bruyères le Châtel with authorised atmospheric releases. A small fraction of the tritium released entered into environmental samples under three forms: (i) as part of free water (TFWT - Tissue Free Water Tritium), or associated with organic matter in two ways; either (ii) bound to the oxygen and nitrogen atoms of the material as exchangeable organically bound tritium (E-OBT), or (iii) bound to carbon atoms as non exchangeable organically bound tritium (NE-OBT). The first two components provide only a picture of atmospheric tritium concentrations at the sampling time as they are in equilibrium with atmospheric moisture and soil humidity. Unlike these exchangeable forms, however, NE-OBT is tightly bound to the organic matter and provides an integrated record of atmospheric tritium during the growing phase of the vegetation. We mapped NE-OBT in tree leaf samples in an area of about 25 × 30 km² around the centre of the CEA site and compared the results with those obtained during a previous sampling exercise in 1989. At this time, the activity levels were almost ten times higher than those observed presently in a similar area almost 20 years later which is consistent with the decrease of atmospheric releases issued from the centre. As the activity levels are now close to environmental background specific attention was also paid to the analytical procedure to ensure reliable low level NE-OBT detection.     

Medical radioisotopes in the environment – following the pathway from patient to river sediment

Motivated by the detection of ¹³¹I in river sediment in routine long-term surveillance samples, a systematic short-term study of the wastewater treatment chain was planned and conducted. Inflow, effluent and primary sludge were collected on a daily basis during two weeks at a regional wastewater treatment plant. Samples were investigated by gamma spectroscopy. Four medically used isotopes could be identified (¹³¹I and ^99mTc regularly, ¹⁵³Sm and ¹²³I sporadically). The concentration levels coincide well with literature data for ¹³¹I, and with our own long-term data for ¹³¹I and ^99mTc for the same plant. Cosmogenic ⁷Be activity in primary sludge correlated well with rainfall intensity. Surface sediment was sampled at low tide at both shores of the river, up- and downstream of the plant. ¹³¹I was identified in all samples, with a sharp maximum (about 100 Bq kg⁻¹ d.m.) at the discharge point of the plant and lower levels elsewhere, decreasing monotonically in downstream direction. ⁷Be and ¹³⁷Cs showed the same behaviour, but no peak at the discharge point. Predictions from simple equilibrium models for the transport and sedimentation of ¹³¹I show good agreement with the experimental data and suggest that the wastewater treatment plant is the main source for this isotope.     

Short-term seasonal variability in Be wet deposition in a semiarid ecosystem of central Argentina

The ⁷Be wet deposition has been intensively investigated in a semiarid region at San Luis Province, Argentina. From November 2006 to May 2008, the ⁷Be content in rainwater was determined in 58 individual rain events, randomly comprising more than 50% of all individual precipitations at the sampling period. ⁷Be activity concentration in rainwater ranged from 0.7 ± 0.3 Bq l⁻¹ to 3.2 ± 0.7 Bq l⁻¹, with a mean value of 1.7 Bq l⁻¹ (sd = 0.53 Bq l⁻¹). No relationship was found between ⁷Be content in rainwater and (a) rainfall amount, (b) precipitation intensity and (c) elapsed time between events. ⁷Be ground deposition was found to be well correlated with rainfall amount (R = 0.92). For the precipitation events considered, the ⁷Be depositional fluxes ranged from 1.1 to 120 Bq m⁻², with a mean value of 32.7 Bq m⁻² (sd = 29.9 Bq m⁻²). The annual depositional flux was estimated at 1140 ± 120 Bq m⁻² y⁻¹. Assuming the same monthly deposition pattern and that the ⁷Be content in soil decreases only through radioactive decay, the seasonal variation of ⁷Be areal activity density in soil was estimated. Results of this investigation may contribute to a valuable characterization of ⁷Be input in the explored semiarid ecosystem and its potential use as tracer of environmental processes.     

Laboratory studies of the diffusive transport of Cs and Co through potential waste repository soils

Tests using reconstituted samples have been performed to assess the diffusive transport of ¹³⁷Cs and ⁶⁰Co through natural regolith materials from a region in South Australia being considered for a radioactive waste repository. A double diffusion cell apparatus made of polycarbonate resin was developed to estimate the effective diffusion (D_e) and sorption coefficients (K_d) that allowed large withdrawals from the source and collector cells and has enabled tests with low concentrations of radioactivity. An alternative to porous stainless steel filter plates has also been used to reduce uncertainty in test interpretation. Analysis of the transient data used a staged method of the Laplace transform to take into consideration the volume of the samples withdrawn from the apparatus during testing. At test completion samples were cut into slices and analysed for radionuclide concentration. Data obtained from the sliced samples confirmed that both numerical and experimental data produced acceptable mass balance. The D_e values obtained in this study were of the order of 10⁻⁶ cm² s⁻¹ for both species, higher than previously published data. The K_d values from the diffusion and batch sorption tests were in reasonable agreement for ¹³⁷Cs, but an order of magnitude different for ⁶⁰Co. The sorption of the latter radionuclide was strongly pH dependent, and this dependency during diffusion tests would benefit from further investigation.     

CO2 dispersion around two PWR nuclear power plants in Brazil

Atmospheric air samples were taken within 3 km from power plants encompassing five different distances and wind directions. Samples were taken between 2002 and 2005 aiming to evaluate the environmental ¹⁴C enrichment due to the operation of Brazilian nuclear power plants. The sampling system consisted of a pump connected to a trapping column filled with a 3 M NaOH solution. The trapped CO₂ was analyzed for ¹⁴C by using a single stage accelerator mass spectrometry (SSAMS).     

Depth profile of ²³⁶U/²³⁸U in soil samples in La Palma, Canary Islands

The vertical distribution of the ²³⁶U/²³⁸U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the ²⁴⁰Pu/²³⁹Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA^® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios ²³⁶U/²³⁸U, ²⁴⁰Pu/²³⁹Pu and ²³⁶U/²³⁹Pu, respectively. The ²³⁶U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated a global fallout signature we assume the same origin as the probable source for ²³⁶U. Our measured ²³⁶U/²³⁹Pu value of around 0.2 is within the expected range for this contamination source.     

The simulation of long-range transport of ¹³⁷Cs from East Asia to Japan in 2002 and 2006

To evaluate the quantities of ¹³⁷Cs from past nuclear tests being transported to and deposited in Japan by naturally-occurring phenomena, the authors developed long-range transport models for ¹³⁷Cs considering Asian dust. The simulation using these models backed the observed recent increase of ¹³⁷Cs deposition along the coast of the Sea of Japan in early spring. For the sake of public safety, it is vital to ascertain whether an increase of radioactive deposition is caused by natural phenomena or a nuclear accident. The observations in recent years have suggested that dust and soil containing ¹³⁷Cs is transported from the regions around Inner Mongolia to Japan by the wind. In this paper, using observation data from the early spring of 2002 and 2006, the authors have found good agreement between the simulations and the measurements. The simulations reproduced the entrainment of ¹³⁷Cs and subsequent transport to Japan caused by strong winds associated with low pressure areas around the Inner Mongolian grasslands. The most likely cause of high-level ¹³⁷Cs deposition over northern Japan during March 2002 was ¹³⁷Cs associated with particles transported at low-altitude (1 km) and subjected to precipitation on the 22nd to 24th.     

Statistical characteristics of radionuclide concentration field around a nuclear power plant

A Markov chain model with two states is used for investigating the space and time structure of the concentration field around an elevated continuous source. The concentration field is computed with a time-dependent Gaussian puff dispersion model run with observed meteorological data as input. Spatial distributions of transition probability, Besson persistence coefficient and order of Markov chain are presented for tritium routinely released from a nuclear power plant located about 100 miles east of Bucharest, Romania.