A study of the atmospheric dispersion of a high release of krypton-85 above a complex coastal terrain, comparison with the predictions of Gaussian models (Briggs, Doury, ADMS4)

Atmospheric releases of krypton-85, from the nuclear fuel reprocessing plant at the AREVA NC facility at La Hague (France), were used to test Gaussian models of dispersion. In 2001-2002, the French Institute for Radiological Protection and Nuclear Safety (IRSN) studied the atmospheric dispersion of 15 releases, using krypton-85 as a tracer for plumes emitted from two 100-m-high stacks. Krypton-85 is a chemically inert radionuclide. Krypton-85 air concentration measurements were performed on the ground in the downwind direction, at distances between 0.36 and 3.3 km from the release, by neutral or slightly unstable atmospheric conditions. The standard deviation for the horizontal dispersion of the plume and the Atmospheric Transfer Coefficient (ATC) were determined from these measurements. The experimental results were compared with calculations using first generation (Doury, Briggs) and second generation (ADMS 4.0) Gaussian models. The ADMS 4.0 model was used in two configurations; one takes account of the effect of the built-up area, and the other the effect of the roughness of the surface on the plume dispersion. Only the Briggs model correctly reproduced the measured values for the width of the plume, whereas the ADMS 4.0 model overestimated it and the Doury model underestimated it. The agreement of the models with measured values of the ATC varied according to distance from the release point. For distances less than 2 km from the release point, the ADMS 4.0 model achieved the best agreement between model and measurement; beyond this distance, the best agreement was achieved by the Briggs and Doury models.     

A new compilation of the atmospheric 85krypton inventories from 1945 to 2000 and its evaluation in a global transport model

This paper gives the yearly (85)Kr emissions of all known reprocessing facilities, which are the main sources of (85)Kr in the atmosphere since 1945, for the years 1945 until 2000. According to this inventory 10,600 PBq (Peta=10(15)) of (85)Kr have been globally emitted from the year 1945 until the end of 2000. The global atmospheric inventory at the end of the year 2000 amounts to 4800 PBq. These emissions have been incorporated into the ECHAM4 atmospheric general circulation model as point sources. Monthly mean model results are compared with measurements made at different locations and times. The influence of each source on the measured concentrations at various locations is studied. The calculated concentrations are found to give reasonably good agreement with the observations, indicating that the emission inventory is realistic. Although, at all northern hemispheric observation sites the model tends to slightly overestimate the concentrations. A possible reason for this overestimation can be found in model features (coarse resolution in time and space). The most prominent discrepancy that is consistently repeated at all northern hemispheric stations occurs in the early 1990s. This could most likely be related to an overestimate of sources. Possibly, the Russian emissions declined earlier than assumed in the current database. Another discrepancy between observations and simulations indicating an incompleteness of the release data is found at some southern hemispheric sites. The variability of their observations could only be explained by regional sources. However, several spikes occur after 1992 when no reprocessing facility is known to be in operation in the southern hemisphere. Production of isotopes for radiopharmaceuticals like technetium-99m from highly enriched uranium is the most likely explanation.     

Krypton-85 in the atmosphere 1950–1977: a data review

For over 20 years the radioactive noble gas ⁸⁵Kr, the product of nuclear industry, has been released to the environment mainly from nuclear fuel reprocessing plants. Owing to its relatively long half-life $\text{T(}\text{1}\text{2}\text{= 10.76}\text{y}\text{)}$ and the absence of other appreciable sinks, a cumulative buildup of ⁸⁵Kr in the atmosphere is observed. The mean ⁸⁵Kr surface air activity in the northern hemisphere has increased from about 20 dpm/mmol Kr in 1950 to about 750 dpm/mmol Kr in 1977. In recent years, a substantial slow-down of the ⁸⁵Kr emission rate to the atmosphere has been observed. The published data indicate rather good mixing of ⁸⁵Kr in the northern hemisphere, but a gradient is observed in the southern hemisphere due to the fact that all nuclear fuel reprocessing plants are situated in the northern hemisphere and due to poor mixing of the atmosphere in the meridional direction.This paper summarizes nearly all of the data on ⁸⁵Kr activity in the atmosphere published up to the middle of 1978. The spatio-temporal distribution of ⁸⁵Kr atmospheric activity is discussed. Some forecasts of future ⁸⁵Kr concentration in the atmosphere and its possible ecological consequences are also presented.     

Simulating mesoscale transport and diffusion of radioactive noble gases using the Lagrangian particle dispersion model

In order to simulate the impact of mesoscale wind fields and to assess potential capability of atmospheric Lagrangian particle dispersion model (LPDM) as an emergency response model for the decision supports, two different simulations of LPDM with the mesoscale prognostic model MM5 (Mesoscale Model ver. 5) were driven. The first simulation of radioactive noble gas ((85)Kr exponent) emitted during JCO accident occurred from 30 September to 3 October 1999 at Tokai, Japan showed that the first arriving short pulse was found in Tsukuba located at 60km away from the accidental area. However, the released radioactive noble gas was transported back to the origin site about 2 days later due to the mesoscale meteorological wind circulation, enhancing the levels of (85)Kr with the secondary peak in Tsukuba. The second simulation of atmospheric dilution factors (the ratio of concentration to the emission rate, chi/Q), during the underground nuclear test (UNT) performed by North Korea showed that high chi/Q moved to the eastward and extended toward southward in accordance with the mesoscale atmospheric circulations generated by mesoscale prognostic model MM5. In comparison with the measurements, the simulated horizontal distribution patterns of (85)Kr during the JCO are well accord with that of observation in Tsukuba such as the existence of secondary peak which is associated with the mesoscale circulations. However, the simulated level of (85)Kr anomaly was found to be significantly lower than the observations, and some interpretations on these discrepancies were described. Applications of LPDM to two mesoscale emergency response dispersion cases suggest the potential capability of LPDM to be used as a decision support model provided accurate emission rate of accident in case of a large accident.     

Evaluation of radioxenon releases in Australia using atmospheric dispersion modelling tools

The origin of a series of atmospheric radioxenon events detected at the Comprehensive Test Ban Treaty Organisation (CTBTO) International Monitoring System site in Melbourne, Australia, between November 2008 and February 2009 was investigated. Backward tracking analyses indicated that the events were consistent with releases associated with hot commission testing of the Australian Nuclear Science Technology Organisation (ANSTO) radiopharmaceutical production facility in Sydney, Australia. Forward dispersion analyses were used to estimate release magnitudes and transport times. The estimated ¹³³Xe release magnitude of the largest event (between 0.2 and 34 TBq over a 2 d window), was in close agreement with the stack emission releases estimated by the facility for this time period (between 0.5 and 2 TBq). Modelling of irradiation conditions and theoretical radioxenon emission rates were undertaken and provided further evidence that the Melbourne detections originated from this radiopharmaceutical production facility. These findings do not have public health implications. This is the first comprehensive study of atmospheric radioxenon measurements and releases in Australia.     

A performance estimate for the detection of undeclared nuclear-fuel reprocessing by atmospheric 85Kr

To test the sensitivity of using atmospheric (85)Kr to detect undeclared separation of plutonium from irradiated nuclear-reactor fuel, measurements of atmospheric (85)Kr taken in Tsukuba, Japan are analyzed to determine: (1) a lower limit of detection for discovering anthropogenic (85)Kr emissions, (2) the probability of detecting plutonium separation at the Tokai Reprocessing Plant, and (3) the extent to which these results can be generalized to other sites. A LLD of at least 3.4 sigma=0.14 Bq/m(3) with a theoretical false-positive rate of 0.05% is recommended for safeguards' purposes. At this threshold, the continuous separation of 100, 300, and 900 g equivalent weapon-grade plutonium per day was found to correspond to 10%, 50%, and 80% probability of detection, respectively. The smallest detected concentration was for the continuous separation of 45 g/day, with a probability of detection of about 0.6%. It was found that the detection rate is determined predominantly by the weather.     

Assessing and managing the risks of accidental releases of hazardous gas: A case study of natural gas wells contaminated with hydrogen sulfide

Natural gas wells contaminated with the toxic gas hydrogen sulfide (i.e., sour-gas wells) pose potential health risks to workers and to nearby residents. The health risks are a function of the dose-response relationship of hydrogen sulfide, the likelihood of accidental releases, gaseous emission rates, the nature of releases at the well head, dispersion of the emitted gas, and the characteristics of the population at risk. We discuss each of these factors and present a risk analysis of a hypothetical sour-gas well in the vicinity of Evanston, WY. We found that the greatest risks for life-threatening effects would occur in the northwest downwind sector after a horizontal release of gas at the well. Subacute effects (e.g., respiratory irritation) after a vertical release of gas would occur primarily to the northeast. Management of health risks involves the use of techniques for preventing inadvertent releases and methods for limiting population exposures.     

Calculation of the depletion of airborne pollutant plumes through dry deposition processes

The depletion of airborne pollutant plumes resulting from dry deposition on ground surfaces should be taken into account when estimating pollutant concentrations in air at distances downwind from their sources. This can be done by using a reduced release rate instead of the actual release rate for the pollutant in atmospheric dispersion equations. The reduced release rate is the actual rate of release multiplied by a depletion fraction. Depletion fractions for use with the Gaussian atmospheric dispersion equation of Pasquill and Gifford were calculated by numerical integration for downwind distances ranging from 35 to 90 000 m for release heights from 1 to 400 m, and they are tabulated for convenient interpolation for intermediate values of distance and release height. Pasquill atmospheric stability categories A-G are included. The listed values are for a deposition velocity of 0.01 m/s and a wind speed of 1 m/s but can be easily converted to apply to other deposition velocities and wind speeds. The tabulated values may be applied for downwind distances close enough to the point of release that the Gaussian model may be assumed to be realistic and where the vertical dispersion of the plume has not yet been significantly affected by the overlying atmospheric lid.     

Carbon-14 discharges from the nuclear fuel cycle: 2. Local effects

Environemtnal ¹⁴C levels around various types of nuclear installations within the UK have been monitored during recent years. Enhanced ¹⁴C levels have been detected around both the nuclear fuel reprocessing plant as Sellafield and the thermal nuclear power station complex at Hunterston. From these measurements, the radiological impact of the ¹⁴C discharges on the local population is assessed. It is conservatively estimated that the ¹⁴CO₂ emissions from Sellafield between 1952 and 1985 could have delivered an 8·4 man Sv collective effective dose equivalent commitment to the population living within 40 km of the site. The maximum possible collective dose to the population within 15 km of Hunterston in 1984 was 15 × 10⁻³ man Sv. Conservative estimates of maximum annual effective dose equivalents to individuals around Sellafield and Hunterston are 0·2 mSv (in 1982) and 12 μSv (in 1984), respectively. These dose levels do not exceed the limits recommended by ICRP but the former value clearly indicates that, for the larger discharges at least, consideration and optimisation of ¹⁴C releases are fully justified. The same ¹⁴C measurements are also used to test the validity of two atmospheric dispersion models, the Gaussian plume and the so-called ‘hyperbolic’ models. The former is excellent in predicting downwind ¹⁴C levels around Hunterston but is unsatisfactory when applied to Sellafield, whereas the latter proves reliable at both sites. Further investigations suggest that the Gaussian plume model's poor performance at Sellafield can be explained by inaccurate input data.     

85Kr atmospheric concentration in Bratislava from 1980 to 1983

A cryogenic-chromatographic method for determination of ⁸⁵Kr in the atmosphere is presented. Sampling of the air on the activated-charcoal, chromatographic separation of Krypton from the other air components and radioactivity measurement are described in details. The activity of ⁸⁵Kr is measured by small proportional counters with sensitive volumes of 5 and 10 cm³. Results of the measurements of ⁸⁵Kr air concentration in Bratislava from 1980 to 1983 are presented and compared with other ⁸⁵Kr data measured in Europe.     

Variation of short-lived beta radionuclide (radon progeny) concentrations and the mixing processes in the atmospheric boundary layer

Radon is emitted to the atmosphere with quasi constant emission rates depending on the radium concentration in the earth's crust and soil physical properties. In this way, the ²²²Rn and ²²⁰Rn concentration in air reflects significantly the thickness of the atmospheric boundary layer (ABL). The aerosol-associated, beta-emitting progeny nuclides of ²²²Rn were measured daily in the framework of the atmospheric radioactivity monitoring program of NIMH at Sofia. The ²¹⁴Pb concentration was estimated from the measured short-lived beta activity of 24-h filter samples, changed daily at 6:00 GMT. The impact of some meteorological factors such as wind direction, wind velocity, humidity, and temperature on short-lived beta radionuclides is estimated, and the results show no simple statistical relationship. A seasonal pattern was observed with winter minima and late summer-early autumn maxima. High variability in daily morning concentrations and mean monthly values was observed. There were well pronounced differences between years. The height of the convective ABL was estimated from daily radio-soundings at 12:00 GMT for the period 2001-2006 and from seven soundings per day during the experimental campaign in Sofia in October 2003. In general, concentrations of short-lived ²²²Rn progeny nuclides decreased with increased convective ABL height.     

An improved method for Kr analysis by liquid scintillation counting and its application to atmospheric Kr determination

Atmospheric ⁸⁵Kr concentration at Fukuoka, Japan was determined by an improved ⁸⁵Kr analytical method using liquid scintillation counting (LSC). An average value of 1.54 ± 0.05 Bq m⁻³ was observed in 2008, which is about two times that measured in 1981 at Fukuoka, indicating a 29 mBq y⁻¹ rate of increase as an average for these 27 years. The analytical method developed involves collecting Kr from air using activated charcoal at liquid N₂ temperature and purifying it using He at dry ice temperature, followed by Kr separation by gas chromatography. An overall Kr recovery of 76.4 ± 8.1% was achieved when Kr was analyzed in 500-1000 l of air. The Kr isolated by gas chromatography was collected on silica gel in a quartz glass vial cooled to liquid N₂ temperature and the activity of ⁸⁵Kr was measured with a low-background LS counter. The detection limit of ⁸⁵Kr activity by the present analytical method is 0.0015 Bq at a 95% confidence level, including all propagation errors, which is equivalent with ⁸⁵Kr in 1.3 l of the present air under the analytical conditions of 72.1% counting efficiency, 0.1597 cps background count rate, and 76.4% Kr recovery.     

Apparent 85Kr ages of groundwater within the Royal watershed, Maine, USA

Specific 85Kr activity is mapped from 264 domestic and municipal wells sampled during 2002-2004 in the Royal watershed (361 km2), Maine. Gas samples are collected at 20 m, 40 m, and > 50 m interval depths within the unconfined aquifers. Gas extraction for 85Kr from wells is obtained directly via a wellhead methodology avoiding conventional collection of large sample volumes. Atmospheric 85Kr input to the recharge environment is estimated at 1.27 Bq m(-3) by time-series analyses of weighted monthly precipitation (2001-2004). Numerical simulation of Kr gas transport through the variable unsaturated zones to the water table suggests up to 12-year time lags locally, thus biasing the 85Kr groundwater ages. Apparent 85Kr ages suggest that approximately 70% of groundwater near 20 m depth was recharged less than 30 years BP (2004). Mass-age transport modeling suggests that post mid-1950s recharge penetrates to part of the basin's floor and that older groundwater seeps from the underlying fractured bedrock may occur.     

Carbon-14 transfer into rice plants from a continuous atmospheric source: observations and model predictions

Carbon-14 ((14)C) is one of the most important radionuclides from the perspective of dose estimation due to the nuclear fuel cycle. Ten years of monitoring data on (14)C in airborne emissions, in atmospheric CO(2) and in rice grain collected around the Tokai reprocessing plant (TRP) showed an insignificant radiological effect of the TRP-derived (14)C on the public, but suggested a minor contribution of the TRP-derived (14)C to atmospheric (14)C concentrations, and an influence on (14)C concentrations in rice grain at harvest. This paper also summarizes a modelling exercise (the so-called rice scenario of the IAEA's EMRAS program) in which (14)C concentrations in air and rice predicted with various models using information on (14)C discharge rates, meteorological conditions and so on were compared with observed concentrations. The modelling results showed that simple Gaussian plume models with different assumptions predict monthly averaged (14)C concentrations in air well, even for near-field receptors, and also that specific activity and dynamic models were equally good for the prediction of inter-annual changes in (14)C concentrations in rice grain. The scenario, however, offered little opportunity for comparing the predictive capabilities of these two types of models because the scenario involved a near-chronic release to the atmosphere. A scenario based on an episodic release and short-term, time-dependent observations is needed to establish the overall confidence in the predictions of environmental (14)C models.     

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.     

Monitoring iodine-129 in air and milk samples collected near the Hanford Site: an investigation of historical iodine monitoring data

While other research has reported on the concentrations of (129)I in the environment surrounding active nuclear fuel reprocessing facilities, there is a shortage of information regarding how the concentrations change once facilities close. At the Hanford Site, the Plutonium-Uranium Extraction (PUREX) chemical separation plant was operating between 1983 and 1990, during which time (129)I concentrations in air and milk were measured. After the cessation of chemical processing, plant emissions decreased 2.5 orders of magnitude over an 8-year period. An evaluation of (129)I and (127)I concentration data in air and milk spanning the PUREX operation and post-closure period was conducted to compare the changes in environmental levels. Measured concentrations over the monitoring period were below the levels that could result in a potential annual human dose greater than 1 mSv. There was a measurable difference in the measured air concentrations of (129)I at different distances from the source, indicating a distinct Hanford fingerprint. Correlations between stack emissions of (129)I and concentrations in air and milk indicate that atmospheric emissions were the major source of (129)I measured in environmental samples. The measured concentrations during PUREX operations were similar to observations made around a fuel reprocessing plant in Germany. After the PUREX Plant stopped operating, (129)I concentration measurements made upwind of Hanford were similar to the results from Seville, Spain.     

Association of plutonium with sediments from the Ob and Yenisey Rivers and Estuaries

The present study applied sequential extraction techniques to investigate the binding and mobility of plutonium (Pu) in sediments from the rivers and estuaries of the Ob and Yenisey. As a study site, the Ob and Yenisey are particularly interesting as both rivers have weapons-grade Pu sources in their catchment areas, including the Russian Pu production and reprocessing plants at Mayak, Tomsk-7 and Krashnoyarsk, and the Semipalantinsk nuclear weapons testing site in Kazakhstan. Plutonium activity and ²⁴⁰Pu/²³⁹Pu ratios were determined using accelerator mass spectrometry (AMS). Sequential extractions showed that between 47 and 80% of the Pu in Yenisey River sediments and 35–53% of the Pu in soils around the Techa River are mobilized with weak oxidising agents, which can indicate that Pu is bound to organic material. In contrast, Pu in Ob and Yenisey Estuarine sediments was more strongly bound, with 60–100% being found in the HNO₃-extractable fraction. This change in speciation could reflect either that Pu bound to organic material in the Techa and Yenisey River sediments becomes more fixed to the sediments with time, or that organic-bound Pu is mobilized and released to the water when the sediments encounter the more saline water of the Ob and Yenisey estuaries. In general, ²⁴⁰Pu/²³⁹Pu ratios were relatively consistent between different extraction fractions, although, in whole sediments, an increase in ratio was observed with distance from the source. This reflects the increased influence of weapon fallout from catchment runoff within the river systems, as compared to the weapons-grade sources close to the production and reprocessing plants. Knowledge of Pu speciation in the Ob and Yenisey Rivers, and the processes controlling its behaviour in estuarine systems, can improve predictions of its transfer and subsequent environmental impact to Arctic Seas.     

Biologically induced Po emission from fresh water

Behavior of Po in fresh waters was examined in laboratory culture experiments using fresh water collected from a small pool, Xi river and Xiqing lake, showing formation of volatile Po compounds followed by emission to air. Addition of tryptone to the fresh water cultures increased the emission of Po considerably along with a growth of microorganisms, suggesting a connection of chemoheterotrophs to Po emission. Participation of photoautotrophs was also considered because Po emission was increased when NaHCO3 was added to the fresh water cultures. The emission behavior of Po and S in these experiments appeared in different ways. The quantity of Po emitted was comparable to the previous culture experiments (Momoshima, Song, Osaki & Maeda, Environ. Sci. Technol., 35, 2956-2960, 2001) in which artificial culture medium containing 3% NaCl was used and inoculated with sea sediment extract. The biological support for Po emission, thus, would be a general phenomenon in fresh water as well as a seawater environment and is possibly a source for atmospheric Po.     

Conclusions on plutonium separation from atmospheric krypton-85 measured at various distances from the Karlsruhe reprocessing plant

For wide-area atmospheric monitoring, krypton-85 is the best indicator for clandestine plutonium separations. The detection and false alarm rates were determined from weekly samples at five different distances from the Karlsruhe reprocessing plant between 1985 and 1988. The detection rate for the separation of 4 kg of plutonium per week was found to be as high as 80-90% at a distance of less than 1 km, 70% at 5 km, 40% at 39 km, and 15% at 130 km. At distances up to 40 km, the false alarm rate is less than 3.5%. On average, the fuel released 28 TBq krypton-85 per kg plutonium. For weapons-grade plutonium, the krypton signal would be lower by a factor of 2. Hence, the given percentages correspond to the detection probabilities for the separation of a significant quantity (8 kg) of plutonium per weekly sample under the specific meteorological conditions of the WAK. The minimum separation rates that could have been detected are 2 gram of weapons-grade plutonium per week at a distance of less than 1 km, 40 g/week at 5 km, 200 g/week at 39 km, and 1000 g/week at 130 km.     

Anguilla anguilla L. Genotoxic responses after in situ exposure to freshwater wetland (Pateira de Fermentelos, Portugal)

Pateira de Fermentelos is a Cértima River enlargement, close to its river mouth (by the Agueda River), where the introduction of agricultural chemicals such as fertilisers and pesticides, domestic sewage, as well as heavy metals from electroplating industries, results in increased water pollution. The present research work concerns a 48 h in situ exposure of caged eels (Anguilla anguilla L.) at the Pateira de Fermentelos. Five exposure sites were selected, i.e., site A, site B, site C, site D and site E in order to study its water genotoxicity potential, measured in gill, blood, liver and kidney as DNA strand breaks. Eels were also exposed at a reference site by the Cértima River spring. Bottom water samples were collected for further physical-chemical analysis. Site A exposure, significantly decreased gill, blood and liver DNA integrity. Gill and liver DNA integrity was also significantly decreased at site B. At site C only blood DNA integrity was significantly decreased. The present field in situ study demonstrated that the three exposure sites close to the Pateira initial part, such as A, B and C are polluted by pro and/or genotoxic compounds. The genotoxic effects induced in A. anguilla L. suggest a different contamination of the exposure sites A, B and C, in genotoxic chemicals. Thus, according to its genotoxic potential the exposure sites A, B and C, may be ordered as follows site A>site B>site C. No genotoxic effects on A. anguilla L. were observed at site E as DNA strand breaks increase.