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.     

Probabilistic risk assessment for long-range atmospheric transport of radionuclides

A simplified means of probabilistic risk assessment (PRA) for long-range atmospheric transport based on a K-diffusion model is presented. In a case study, model parameters are estimated by comparing with the results of long-range atmospheric dispersion model calculations using one-year numerical weather prediction model data. It is found that the estimated ensemble mean provides a reasonable first approximation to the total dry and wet deposition from the one-year continuous release.     

Soil mutagenicity as a strategy to evaluate environmental and health risks in a contaminated area

Soil can be a storage place and source of pollutants for interfacial environments. This study looked at a site contaminated with wood preservatives as a source of mutagens, defined routes and extent of the dispersion of these contaminants by particle remobilization and atmospheric deposition, considering an evaluation of risk to human health by quantifying mutagenic risk. Soil sampling sites were chosen at gradually increasing distances (150, 500 and 1700 m) from SI (industrial area pool) and indoor dust (pool in an area at risk at 385 m and at 1700 m). Mutagenesis was evaluated in the Salmonella/microsome assay, TA98, TA97a and TA100 strains with and without S9 mix, YGs strains 1041, 1042 and 1024 for nitrocompounds. Acid extracts were analyzed to define the effects of metals and organics for polycyclic aromatic hydrocarbons (PAHs) and nitroderivates, besides concentrations of these compounds and pentachlorophenol (PCP). Risk to human health was obtained from the relation between the quantified potential of mutagenic risk and estimated soil ingestion for children according to USEPA. Metal concentrations showed a gradient of responses with As, Cr and Cu (total metal) or Cr and Cu (fraction available) higher for SI. However, mutagenic effects of the mixtures did not show this grading. Site SR1700, without a response, was characterized as a reference. In organic extracts, the mutagenesis responses showed the mobility of these compounds from the source. In the surrounding area, a smaller pattern similar to SI was observed at SR150, and at the other sites elevated values of direct mutagenesis at SR500 and diminished effects at SR1700. Tests with YG strains indicated that nitrated compounds have a significant effect on the direct mutagenesis found, except SR500. The investigation of indoor dust in the surrounding area enabled confirmation of the particle resuspension route and atmospheric deposition, showing responses in mutagenicity biomarkers, PAH concentrations and PCP dosage similar to SI. The range of values obtained, considering the soil masses needed to induce mutagenicity was 0.02 to 0.33 g, indicating a high risk associated with human populations exposed, since these values found surpass the standard estimate of 200 mg/day of rate of soil ingestion for children according to USEPA. The study showed that it is essential to evaluate the extent of contamination from the soil to delimit remedial measures and avoid damage to the ecological balance and to human health.     

Organically bound tritium (OBT) for various plants in the vicinity of a continuous atmospheric tritium release

In order to quantify tritium impact on the environmental, we studied vegetation continuously exposed to a tritiated atmosphere. We chose lichens as bio-indicators, trees for determination of past tritium releases of the Valduc Centre, and lettuce as edible vegetables for dose calculation regarding neighbourhood. The Pasquill and Doury models from the literature were tested to estimate tritium concentration in the air around vegetable for distance from the release point less than 500m. The results in tree rings show that organically bound tritium (OBT) concentration was strongly correlated with tritium releases. Using the GASCON model, the modelled variation of OBT concentration with distance was correlated with the measurements. Although lichens are recognized as bio-indicators, our experiments show that they were not convenient for environmental surveys because their age is not definitive. Thus, tritium integration time cannot be precisely determined. Furthermore, their biological metabolism is not well known and tritium concentration appears to be largely dependent on species. An average conversion rate of HTO to OBT was determined for lettuce of about 0.20-0.24%h(-1). Nevertheless, even if it is equivalent to values already published in the literature for other vegetation, we have shown that this conversion rate, established by weekly samples, varies by a factor of 10 during the different stages of lettuce development, and that its variation is linked to the biomass derivative.     

Numerical simulation of 137Cs and (239,240)Pu concentrations by an ocean general circulation model

We simulated the spatial distributions and the temporal variations of 137Cs and (239,240)Pu concentrations in the ocean by using the ocean general circulation model which was developed by National Center of Atmospheric Research. These nuclides are introduced into seawaters from global fallout due to atmospheric nuclear weapons tests. The distribution of radioactive deposition on the world ocean is estimated from global precipitation data and observed values of annual deposition of radionuclides at the Meteorological Research Institute in Japan and several observed points in New Zealand. Radionuclides from global fallout have been transported by advection, diffusion and scavenging, and this concentration reduces by radioactive decay in the ocean. We verified the results of the model calculations by comparing simulated values of 137Cs and (239,240)Pu in seawater with the observed values included in the Historical Artificial Radionuclides in the HAM database, which has been constructed by the Meteorological Research Institute. The vertical distributions of the calculated 137Cs concentrations were in good agreement and are in good agreement with the observed profiles in the 1960s up to 250 m, in the 1970s up to 500 m, in the 1980s up to 750 m and in the 1990s up to 750 m. However, the calculated 137Cs concentrations were underestimated compared with the observed 137Cs at the deeper layer. This may suggest other transport processes of 137Cs to deep waters. The horizontal distributions of 137Cs concentrations in surface water could be simulated. A numerical tracer release experiment was performed to explain the horizontal distribution pattern. A maximum (239,240)Pu concentration layer occurs at an intermediate depth for both observed and calculated values, which is formed by particle scavenging. The horizontal distributions of the calculated (239,240)Pu concentrations in surface water could be simulated by considering the scavenging effect.     

Comparison between the predictions of a Gaussian plume model and a Lagrangian particle dispersion model for annual average calculations of long-range dispersion of radionuclides

This study attempts to validate the applicability of a simple Gaussian dispersion model for predicting long-range dispersion of continuous releases from an industrial site, by comparison with a Lagrangian particle dispersion model. The United Kingdom Meteorological Office model NAME has been used to predict annual average concentrations of radionuclides over Western Europe, resulting from discharges from the British Nuclear Fuels (BNFL) site at Sellafield, UK. The results are compared here to calculations performed using a conventional Gaussian type of dispersion model, PLUME. The results of the Gaussian model were compared at 14 locations within Western Europe at long range (up to 1700 km). The differences in predictions between the models were explained readily by differences in the way dispersion and deposition processes are represented in the two models. However, differences are generally small compared to the expected precision of the models. The implementation of environmental processes in NAME is more complete and realistic than in PLUME, and as such the results from this model may be considered more realistic. However, given that PLUME is much simpler to use, and appears to over-estimate, rather than under-estimate, environmental concentrations, its use for radiological assessments appears appropriate.     

The geographic distribution of radionuclide deposition across the continental US from atmospheric nuclear testing

For the first time, calculations for the more than 3000 counties of the US have been completed that estimate the average deposition density (Bq m(-2)) of more than 40 radionuclides in fallout from atmospheric nuclear weapons tests conducted in the US (1951-1962) and 19 radionuclides from tests conducted elsewhere in the world (1952-1963). The geographic pattern of deposition across the US, as well as the amount of fallout deposited, varied significantly depending on whether the tests were conducted within or outside of the US. Fallout deposited from the Nevada Test Site (NTS) varied geographically as a result of dispersion and dilution in the atmosphere, the wind patterns following each test, and the occurrence of localized rainfall events. In general, states immediately east of the NTS received the highest deposition from tests conducted there. In contrast, the variation in deposition across the country from global fallout was less than for NTS fallout primarily reflecting variations in annual precipitation across larger regions. Hence, in the eastern and mid-western US, where rainfall is above the national average, higher levels of global fallout were deposited than in the more arid southwestern states. This paper presents a summary of the methods used and findings of our studies on fallout from NTS and global fallout, with emphasis on two of the most important radionuclides, (131)I and (137)Cs.     

基于环境承载力的京津冀雾霾治理政策效果评估

雾霾污染治理是京津冀协同发展需要解决的重大问题。2013年9月颁布的"大气污染防治行动计划(大气国十条)"明确提出了京津冀地区雾霾治理目标,各地区也制定了雾霾污染治理的政策措施。本文旨在环境承载力分析的基础上评估雾霾治理的政策效果。首先,分析了京津冀地区大气环境污染特征,并结合相关文献确定京津冀地区雾霾治理的主要影响因素为污染物排放、风力以及相邻地区的传输效应等;其次,将影响PM_(2.5)浓度主要因素进行统计建模,并采用分位数回归模型进行矫正,大大提高模型的拟合精度;再次,基于大气国十条规定的京津冀各地区的PM_(2.5)年均浓度目标计算各地区的大气环境承载力;最后,在假定风力等气象条件不变的情况下,根据大气国十条规定的京津冀地区的污染物排放量利用统计模型模拟2017年的雾霾污染水平,模拟除张家口、承德和秦皇岛以外其余10个地区年均浓度60μg/m~3和70μg/m~3目标下PM_(2.5)日均浓度发生频率的变化情况,评估和讨论大气国十条提出的京津冀雾霾治理目标。结果表明:按照大气国十条减排计划的京津冀地区污染物排放量普遍高于其PM_(2.5)浓度目标下的大气环境容量(邯郸市除外),即大气国十条所规定的减排措施难以实现既定的PM_(2.5)浓度目标;PM_(2.5)年均浓度目标从60μg/m~3上升到70μg/m~3,重污染天气发生频率上升有限,大气污染物的减排量却显著下降。因此,要实现既定的雾霾浓度控制目标,天津和河北需要进一步加大污染物减排力度;雾霾治理应注重减少重污染天气的发生频率,治理重点应转向重度雾霾发生频率较高的冬季污染物排放控制;在科学确定环境承载力的基础上,确定切实可行的PM_(2.5)浓度控制目标,制定具有可操作性的污染物减排计划。     

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.     

Reconstruction of atmospheric concentrations and deposition of uranium and decay products released from the former uranium mill at Uravan, Colorado

Radionuclide concentrations in air from uranium milling emissions were estimated for the town of Uravan, Colorado, USA and the surrounding area for a 49-yr period of mill operations beginning in 1936 and ending in 1984. Milling processes with the potential to emit radionuclides to the air included crushing and grinding of ores; conveyance of ore; ore roasting, drying, and packaging of the product (U(3)O(8)); and fugitive dust releases from ore piles, tailings' piles, and roads. The town of Uravan is located in a narrow canyon formed by the San Miguel River in western Colorado. Atmospheric transport modeling required a complex terrain model. Because historical meteorological data necessary for a complex terrain model were lacking, meteorological instruments were installed, and relevant data were collected for 1 yr. Monthly average dispersion and deposition factors were calculated using the complex terrain model, CALPUFF. Radionuclide concentrations in air and deposition on ground were calculated by multiplying the estimated source-specific release rate by the dispersion or deposition factor. Time-dependent resuspension was also included in the model. Predicted concentrations in air and soil were compared to measurements from continuous air samplers from 1979 to 1986 and to soil profile sampling performed in 2006. The geometric mean predicted-to-observed ratio for annual average air concentrations was 1.25 with a geometric standard deviation of 1.8. Predicted-to-observed ratios for uranium concentrations in undisturbed soil ranged from 0.67 to 1.22. Average air concentrations from 1936 to 1984 in housing blocks ranged from about 2.5 to 6 mBq m(-3) for (238)U and 1.5 to 3.5 mBq m(-3) for (230)Th, (226)Ra, and (210)Pb.     

Measurements of major ion concentration in settled coarse particles and aerosols at a semiarid rural site in India

Deposition rates and deposition velocities of water-soluble ions (F, Cl, NO3, SO4, NH4, Ca, Mg, Na and K) were measured at a rural site (Gopalpura, Agra). Dry deposition samples were collected throughout the year from December 1995 to August 1997, while the aerosol samples were collected only during the winter season of 1996. Surrogate technique was used to collect the dry deposition samples, while aerosol samples were collected on PTFE membrane filter. Deposition velocities (Vd) of SO4 and NO3 are < or = 0.01 m s(-1) while Ca, Mg, Na, K, NH4, F and Cl exhibit greater than 0.01 m s(-1) Equivalent concentration ratios of K/Na, Ca/Na and Mg/Na conform with the corresponding ratios of local soil, indicating the dominant contribution of local sources. Deposition rates are maximum in winter, followed by summer and monsoon. No significant differences are found in dry deposition rates of all ions or in atmospheric concentrations of soil-derived elements with respect to wind direction. However, in aerosols, concentrations of F, Cl, NO3 and SO4 are higher with winds from southwesterly and westerly directions corresponding to pollution sources located in these directions. Deposition data have been used to calculate the critical load of S and N for soil with respect to Triticum vulgaris. The critical load of actual acidity was found to be 622.4 eq ha(-1) year(-1) within the range of 500-1,000 eq ha(-1) year(-1) as assessed by the RAINS-Asia model for this region. The present load of S and N (77.4 and 86.4 eq ha(-1) year(-1)) was much lower than the critical load of S and N (622.4 and 2,000 eq ha(-1) year(-1)), indicating that at present there is no harmful effect on ecosystem structure and function.     

In situ metrology of 85Kr plumes released by the COGEMA La Hague nuclear reprocessing plant

The IRSN (Institut de Radioprotection et de S?reté Nucléaire, France) has started an in situ study of the behaviour of atmospheric releases close-by the COGEMA La Hague nuclear reprocessing plant. The study is designed to improve information on the dispersion of radioactive pollutants very close to the emission point--a 100 m height chimney. In this situation, close to the emission and height of the emission, Gaussian models generally used to predict the behaviour of atmospheric releases are not well adapted. The study is based on the characterisation of the 85Kr emitted during normal operations of the reprocessing process. Temporal and spatial variations of the plume shape were investigated with intensive in situ measurements. Live in situ techniques to measure the electrons and the photons emitted by the 85Kr have been implemented and will be described. Preliminary results showing the interest of the techniques were presented. Variations of the dose rates created by the photon flux of a plume were directly measured and correlated to other quantities.     

Photochemical dispersion modeling: Review of model concepts and applications studies

Over the last decade, the development and application of sophisticated atmospheric models that simulate the transport and dispersion of ozone and its precursors have advanced rapidly. Further advancements are most likely to be found in more complete temporal and spatial characterization of photochemical smog formation processes via measurement. This paper provides an overview of the development of atmospheric photochemical dispersion models, first discussing in general terms the various physical processes occurring in the atmosphere that govern the formation, transport, and ultimate fate of ozone. Procedures for representing these physical processes in mathematical terms are presented next. Nearly all of the photochemical models in use today are derived from the semiempirical atmospheric diffusion equation, though theoretical formulations vary depending on which of the various terms in the pollutant mass balance equation are deemed significant for the application at hand. Examples of recent applications of the range of available photochemical model are presented, together with estimates of the accuracy of each generic modeling concept. Several topics warranting future research are identified, including the need to incorporate explicitly more of the stochastic (or probabilistic) nature of the atmosphere into the form of current photochemical model predictions (i.e., estimates of the variance and higher order moments of the predicted concentration distribution).     

Using radiotracer techniques for coastal hydrodynamic model evaluation

A three-dimensional (3D) water circulation and contaminant transport model of Manila Bay has been developed with the aim of better understanding the formation and movement of harmful algal blooms. Radiotracer techniques were used to evaluate the model by recording the dispersion of a tracer at depths of 2 and 15 m near the injection point. The selected tracer was 99mTc eluted from a molybdenum/technetium medical generator. The rationale for the choice of the tracer and the location of the injection is discussed. At 2 m the transport was dominated by the prevailing winds, and at 15 m by tidally induced currents. The development of the hydrodynamic model and its experimental evaluation were iterative processes. The experimental study confirmed the need for full 3D modelling of Manila Bay; quantified the impact of the prevailing wind field on contaminant dispersion near the injection point; and allowed the calculation of transverse dispersivity to guide the selection of parameter values used in the overall model.     

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.     

Modelling future impacts of air pollution using the multi-scale UK Integrated Assessment Model (UKIAM)

Integrated assessment modelling has evolved to support policy development in relation to air pollutants and greenhouse gases by providing integrated simulation tools able to produce quick and realistic representations of emission scenarios and their environmental impacts without the need to re-run complex atmospheric dispersion models. The UK Integrated Assessment Model (UKIAM) has been developed to investigate strategies for reducing UK emissions by bringing together information on projected UK emissions of SO₂, NO_x, NH₃, PM₁₀ and PM_2.5, atmospheric dispersion, criteria for protection of ecosystems, urban air quality and human health, and data on potential abatement measures to reduce emissions, which may subsequently be linked to associated analyses of costs and benefits. We describe the multi-scale model structure ranging from continental to roadside, UK emission sources, atmospheric dispersion of emissions, implementation of abatement measures, integration with European-scale modelling, and environmental impacts. The model generates outputs from a national perspective which are used to evaluate alternative strategies in relation to emissions, deposition patterns, air quality metrics and ecosystem critical load exceedance. We present a selection of scenarios in relation to the 2020 Business-As-Usual projections and identify potential further reductions beyond those currently being planned.     

Areal distribution of 129I in west cumbrian solis

¹²⁹I has been released during operations at the BNFL nuclear fuel reprocessing plant at Sellafield in west Cumbria over the past thirty years with about 95% being discharged into the sea and 5% into the atmosphere. Soil samples have been taken within a 40 km radius of Sellafield to determine the extent to which the ¹²⁹I is deposited in the immediate vicinity of the plant. The ¹²⁹I content has been determined by a sensitive neutron activation technique and levels in soil were found to be elevated above global levels in all samples. The areal distribution of ¹²⁹I was consistent with direct deposition following release to the atmosphere from Sellafield and the relationship between ¹²⁹I activity and the distance from Sellafield was of a form predicted by atmospheric dispersion models. The absence of any observable return of ¹²⁹I from the sea has implications for assessments of dose.     

Long period study of outdoor radon concentration in Milan and correlation between its temporal variations and dispersion properties of atmosphere

The results of a survey of outdoor radon concentrations in Milan are reported. Measurements were performed hourly over a continuous four year period from January 1997 to December 2000. Radon concentration was obtained by two means: both direct measurement of radon; and measurement of its decay products. The average daily pattern of radon concentration featured a minimum in the late afternoon and a maximum in the early hours of the morning. A seasonal pattern with higher concentrations in winter than in summer (from around 15 Bq m(-3) in winter to around 5 Bq m(-3) in summer) was also observed. Similar average annual values of around 10 Bq m(-3) were obtained. The annual effective outdoor radon dose was found to be 0.12 mSv. The variation from minimum in the afternoon to maximum the following morning was found to be a good indicator of the height of the nocturnal mixing layer. The variation between maximum and minimum levels on the same day is an index of the maximum height of the mixing layer. Furthermore, our long term measurements of radon have permitted us to examine the dispersion characteristics of the atmosphere over Milan, and to establish the frequency of conditions unfavourable to the dispersion of atmospheric pollutants.     

Wet and dry deposition of 129I in Seville (Spain) measured by accelerator mass spectrometry.

Iodine-129 (T1/2 = 1.57 x 10(7) yr) concentrations have been determined by accelerator mass spectrometry in rainwater samples taken at Seville (southwestern Spain) in 1996 and 1997. This technique allows a reduction in the detection limits for this radionuclide in comparison to radiometric counting and other mass spectrometric methods such as ICP-MS. Typical 129I concentrations range from 4.7 x 10(7) 129I atoms/l (19.2%) to 4.97 x 10(9) 129I atoms/l (5.9%), while 129I depositions are normally in the order of 10(8)-10(10) atoms/m2d. These values agree well with other results obtained for recent rainwater samples collected in Europe. Apart from these, the relationship between 129I deposition and some atmospheric factors has been analyzed, showing the importance of the precipitation rate and the concentration of suspended matter in it.